SOVIET ATOMIC ENERGY VOLUME 15, NO. 1
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Volume 15, 'No. I
May, 1964
souiEr
ATOMIC
ENERGY
ATOMHAH 3HEPII4R
.(ATOMNAYA ENERGIYA)
TRANSLATED FROM RUSSIAN
"CONSULTANTS BUREAU
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NUMERICAL METHODS
FOR NOCLEAR:REACTOR
CALCULATIONS-
- by 6.1. Marchuk
THEORY AND ME'TNODS
Of CALCULATING,
NUCLEAR REACTORS,
Edited by G.I. Marchuk
,Gteatest'attention is devoted?to neutron transport theory
and to methods of designing reactors. The general problems
of neutron transport theory are.discussed and special atten-
tion is directed to solving the problem of a point source in an
infinite homogeneous medium.
,.Papers included in the volume discuss such pertinent .?ub-
jects as: the transmission of. a radiation flux near a point
.source - in which the author develops a numerical method
of calculating the radiation field - followed by an analytic
solution of the problem;"an application of the S? method to
"As stated in the foreword, this book is an attempt at a the solution of the neutron transport equations; as 'Well as
tsaic exposition of numerical methods for the calculation, methods of calculating nuclear reactor kinetics, including
of thermal, intermediate and fast neutron-reactors.' The author the placement of.burnable'poisons. Further development of
has admirably succeeded in this goal; his exposition of numerical the theory of resonance neutron capture ?inclUdes such dis= '
methods for reactor calculations 'being the most complete yet cussibns as; numerical methods of'calculating the effective
-published ... The reviewer was impressed with the thoroughness resonance integral in homogeneous uniform, media, and a
and skill bf the author's presentation, The adjoint reactor equa? method of finding,the multi-group cross sections in the
bons are applied throughout the text with originality and effec 'resonance region, a theoretical discussion of the'mathemat-
t
t
tiveness. Similarly, perturbation theory is 'skillfully developed,
while its limitations are clearly recognized and defined. In short,
the book should appeal not only to the applied mathematician,
who is involved in reactor calculations, but also to the general
reactor physicist-or engineer," NUCLEONICS,
completely self-cohtained. He [Marchuk] derives all the
basic equations of reactor theory, develops the most important
approximations, and then shows how the reactor equations (in
their various approximate formsl can be solved numerically .. .
The advantages are clear - The book has many fine features."
NUCLEAR SCIENCE'AND ENGINEERING
rea
-
Ical treatment of nuclear physics experiments, and a
ment' of resonance parameters, nuclear decay times, etc.
The collection employs unified methods of analysis based
on,a strict 'mathematical approach, with a subsequent appli-
cation of the fundamental results to practical solutions.
CONTENTS
Application of the Spherical Harmonics to Transport Theory Prob-
lems: General Properties of the Ph Approximations. .
Application of Spherical Harmonics to Transport Theory Prob-
lems. The P2 Approximation. I `
One,Velocity 'Problem of the Angular Distribution of Neutrons
Emitted by a Point Isotropic Source at the Center of a Sphere.
Spatial and Angular Distribution of the Neutrons from a Point
Source Considering Anisotropic Scattering.
Space-Energy Distribution of-Fast Neutrons in Hydrogen.
The Application of One-Group' Theory to Reactor Calculations.
A-Two-Group Method for Intermediate-Thermal Reactor Calcu-
lations.
Solution of the Kinetic Equations by the S n Method.
Calculatiorf of Poison' Burnup in Reactors.
Thermal Neutron Spectrum in a Homogeneous Mixture of Mod-
erators at Differing Temperatures.
Monte Carlo Calculations of the Energy and Angular Distributions
of y-Quanta Penetrating a Plane-Parallel Layer of Finite Thick-
Neutron Resonance Absorption-in Homogeneous Media.
Effect of Potential and Resonance' Scattering Interference on
Neutron Resonance Absorption.
Neutron Resohance Capture in an Annular Lump.
Method for Constructing Multi-Group Constants in" the Resonance
Region Taking Heterogeneous Effects into Account.
Some Problems in the Statistical Treatment of Nuclear Physics
Measurements.
Optical Model Calculations of the Transport Cross, Section. -
Inelastic Scattering of Neutrons by Iron.
180 pages Translated from Russian,
293 pages ? ' Translated from Russian $60.00'
Entirely devoted to a systematic exposition of numerical
methods of calculation of thermal; intermediate, and fast
neutron reactors. Particular attention is devoted to the
problems of critical mass, the space-energy neutron flux
distribution;, and the neutron importance (iterated fission
probability). The book gives effective methods for reducing
the basic and adjoint reactor equations to a set of multi-
group diffusion 'equations. These equations are then suc-
cessfully solved by the method of difference factorization:
Perturbation theory is used to calculate small effects. Con-
siderable space is devoted to heterogeneous reactor, :calcu-
lations by effective homogenization methods, and in treating
fast-neutron reactors, particular attention is paid to numeri-
cal methods for solving the. kinetic equations. Corresponding
to every set of equations derived, an adjoint set of equations
is also obtained.
While guaranteeing a given accuracy, these calculations
are still sufficiently versatile and' convenient to tie used in
:a wide variety of problems, thus making the book particu-
larly valuable to graduate, students in physics, doctoral
candidates, engineers, and 'scientific workers specializing
in this type of calculation..
CONSULTANTS BUREAU 227 W. 17th St., New York, N. Y. 10011
1 ?
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ATOMNAYA ENERGIYA
EDITORIAL BOARD
A. I. Alikhanov
A. A. Bochvar
N. A. Dollezhal'
K. E. Erglis
V. S. Fursov
I. N. Golovin
V. F. Kalinin
N. A. Kolokol'tsov
(Assistant Editor)
A. K. Krasin
I. F. Kvartskhava
A. V. Lebedinskii
A. I. Leipunskii
M. G. Meshcheryakov
M. D. Millionshchikov
(Editor-in-Chief)
1. 1. Novikov
V. B. Shevchenko
A. P. Vinogradov
N. A. Vlasov
(Assistant Editor)
M. V. Yakutovich
A. P. Zefirov
Vol. 15, No.1
SOVIET ATOMIC
EN-ERGY
A translation of ATOMNAYA ENERGIYA
A publication of the Academy of Sciences of the USSR
61964 CONSULTANTS BUREAU ENTERPRISES, INC.
227 West 17th Street, New York 11, N. Y.
CONTENTS
May, 1964
ENG. I RUSS.
Ion Cyclotron Resonance in a Moving Plasma -I. I. Bakaev, Yu. G. Zalesskii,
N. I. Nazarov, A. M. Ukrainskii, and V. T. Tolok................. .. .... 655 3
The Kinetic Energy of Fragments and Alpha Particles in, the Ternary Fission of U235
-V. N. Dmitriev, K. A. Petrzhak, and Yu. F. Romanov .... .....:..... ...... . 659 6
Distribution of the Number of Counts on a Neutron Detector Placed in a -Reactor
-V. G. Zolotukhin and A. I. Mogil'ner .................... ............. .
Attenuation of Pile Neutron Flux in Polyethylene-V. N. Avaev, G. A. Vasil'ev,
A. P. Veselkin, Yu. A. Egorov, Yu. V. Orlov, and Yu. V. Pankrat'ev .. ............ 671 17
Spectra of Fast Pile Neutrons in Passage Through Polyethylene-V. N. Avaev, G. A. Vasil'ev,
A. P. Veselkin, Yu. A. Egorov, Yu. V. Orlov, and Yu. V. Pankrat'ev .. .... .. .. .. 675 20
The Separation of Zr95, Nb95, and Ru106 from a Mixture of Fission Products by Extraction
with Tributyl Phosphate-N. E. Brezhneva, V. I. Levin, G. V. Korpusov,
E. K. Bogacheva and N. M. Man'ka .................................. 678 23
The Effect of Neutron Irradiation on the Structure and Mechanical Properties of Alloy
Steels-Sh. Sh. Ibragimov, I. M. Voronin, and A. S. Kruglov ................... 685 30
The Corrosive Effect of Fuel Element Solvents on Structural Materials-M. M. Kurtenov
and E. N. Mirolyubov ...........................:............... .
Radiation Dosimeters Based on Thermolumirlescence Measurements in Aluminum Phosphate
Glass (IKS Dosimeters)-I. A. Bochvar. A. A. Vasil'eva, I. B. Keirim-Markus, T. I. Prosina,
Z. M. Syritskaya, and V. V. Yakubik .................................. 704 48
Monitoring Ionizing Radiations Resulting from Nitrogen Reactions-M. T. Dmitriev......... 709 52
LETTERS TO THE EDITOR
Oscillations in a Spatially Nonuniform Plasma in a Magnetic Field-V. G. Davidovskii...... 717 60
New Ways of Increasing the Efficiency of the Microtron-K. A. Belovintsev, A. Ya. Belyak,
V. I. Gridasov, and P. A. Cherenkov ................................... 720 62
Fast Neutron Polarization Apparatus-N. V. Alekseev, U. R. Arifkhanov, N. A. Vlasov,
V. V. Davydov, and L. N. Samoilov .................................. .
The Number of Prompt Neutrons and the Kinetic Energy of Fragments During Low-Energy
Fission of Uzs5-Yu. A. Blyumkina, I. I. Bondarenko, V. F. Kuznetsov, V. G. Nesterov, 725 64
V. N. Okolovich, and G. N. Smirenkin ................................. 725 64
The Optimum Condition for Biological Shielding Against a Number of Radiation Sources
-G. A. Lisochkin ............................................... 729 67
Annual Subscription: $ 95 Single Issue: $30
Single Article: $15
All rights reserved. No article contained herein may be reproduced for any purpose what-
soever without permission of the publisher. Permission may be obtained from Consultants
Bureau Enterprises, Inc., 227 West 17th Street, New York City, United States of America.
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CONTENTS (contin~Qal
The Structure of the Gamma Radiation Field from an Isotropic Point Source in Aluminum
P A G E
ENO. I RUSS.
with Barrier Geometry-V. A. Vorob'ev ?
732
68
The Ratio of the Thermal Neutron Flux in Water to the Power of a Point Source-E. A. Garusov
and Yu. V. Petrov .. . ? a
736
71
..
The Effectiveness of a'System of Absorber Rods Arbitrarily Distributed in a Reflected Reactor
- V. I. Nosov ................................... ...........
737
71
Frequency Analysis in a System which Includes a Runaway Reactor-A. R. Mirzoyan
and I
N
B
ikk
r
.
.
er ........... .......... .. ... ............
741
74
Calculation of the Temperature of Regenerative Preheating of Water in Two-Circuit Atomic
Power Plants-D. Grecov .......................... ..............
744
76
An Investigation of Critical Heat Fluxes During Forced Movement of Monoisopropyl Diphenyl
Heated Below the Saturation Temperature-G.,N. Karavaev, A. D. Leongardt,
and Yu. P. Shlykov ................................... . . ......
747
77
Determination of the Permeability of Pipe Walls with Respect to Helium-I. S. Lupakov,
Yu. S. Kuz'michev, and Yu. V. Zakharov ................ . .............
750
79
The Fluorination of Uranium Sulfate by Chlorine Trifluoride-N. S. Nikolaev
and Yu. D. Shishkov . . . . . . . . . . .. ..............................
753
81
NEWS OF SCIENCE AND TECHNOLOGY
XIII All-Union Conference on Nuclear Spectroscopy-V. P. Rudakov.. . . . . . . . . . . . . . . . .
754
82
Geochemical Conference Dedicated to the Centennial of V. I. Vernadskii - A. I. Tugarinov.. .
755
82
New Trends in Research and Applications for Rare Earths- L, Polyakov .. ..... . . . . . . . ...
758
84
Conference on Nuclear Power Development in the Czechoslovak Socialist Republic
-S. Medonos .................
760
86
Conference of the Plasma Physics Section of the American Physical Society
761
87
Status of the Uranium Industry in the Capitalist Countries as of 1962-V. D. Andreev.
763
88
USAEC Delegation Visits the Soviet Union .............. ...._..... 769
91
BRIEF COMMUNICATIONS ........... .. .. , .. .. ................. 772
93
FROM THE EDITOR
The Introduction of an International System of Units in the USSR-V. Korotkov
... .
774
96
BIBLIOGRAPHY
New Literature ....... ,
. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
A
ti
l
f
h
""""?
779
99
r
c
es
rom
t
e Periodical Literature ........ . .............. ..... . ... . 780
99
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I. I. Bakaev, Yu. G. Zalesskii, N. I. Nazarov,
A. M. Ukrainskii, and V. T. Tolok
Translated from Atomanya Energiya, Vol. 15, No. 1,
pp. 3-6, July, 1963
Original article submitted September 22, 1962
The generation and absorption of ion cyclotron waves in moving plasma bunches was observed. Ab-
sorption of high-frequency power occurred at. two frequencies which were the result of a Doppler shift
in both directions from some mean frequency. It was shown that magnetic beaches play an important
role in the damping of ion cyclotron waves. Thus, in the absence of one beach, the second absorp-
tion peak was not observed. Measurements of the Doppler shift and resonant frequencies made it
possible to determine the mean bunch velocity and the plasma density (6.7 108 cm/sec and 7. 1012
cm-8, respectively).
In most cases, experiments investigating plasma containment in magnetic traps obviously would prefer to work
with plasma at a maximum high temperature. If the plasma is created by means of external sources, there exists the
possibility of additionally heating it before injection into a trap. It is obvious that a sufficiently rapid heating method
is required to heat moving plasma bunches. Ion cyclotron resonance may prove to be such a method.
In fact, no more than 10-5 sec are required for a significant acceleration of plasma ions [1-31 under present-
day conditions for performing experiments on heating a stationary plasma by ion cyclotron resonance. Therefore,
with bunch velocities of the order of 10~ cm/sec, the length of a heating section will have reasonable dimensions
(no more than 1 m). Besides the heating effect, one can probably expect some improvement in the conditions for
ion capture in a magnetic trap because of the increased ion velocity which is directed perpendicularly to the mag-
netic lines of force. Comparing resonance high-frequency heating in stationary and moving plasmas, it is appro-
priate to note still another consideration. In the first case, the plasma completely fills the volume of the dielectric
chamber where the heating must occur. The internal surface of the wall of the cylindrical chamber to which the
coil of the high-frequency circuit is attached is subject to the action of high-frequency electrical discharge since
the electrical field intensity is a maximum at the wall. In such a situation, it is difficult to insure the absence of a
large quantity of impurities from chamber wall materials in the heated plasma.
To'' generator a
I-'1
00003 ?.f hh
Pump. - - ~ - 2 ~_ ~8
00,x, Hydrogen
.W = tax-
V
Fig. 1. Diagram of the experimental apparatus (a) and mag-
netic field topography (b): 1) plasma tube; 2) heating coil;
'3) solenoid; 4) plasma gun.
In the case where there is heating of plasma bunches which are moving ;in a high vacuum along a magnetic
field, it is possible to isolate them from the chamber walls during their time of flight if the cross section of a bunch
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Fig. 2. Oscillogram of the non-resonant loading
introduced into the high-frequency circuit by
a bunch.
vu
0 0
20
o0
10
entering the chamber is less than the cross section of the cham-
ber itself. Further, there is no need for the creation of high-
frequency discharge at the chamber walls since a vacuum no
poorer than 10-7 mm Hg can be maintained in this situation.
If a bunch passes into the high vacuum along the axis of the
heating high-frequency coil so that it doesn't touch the wind-
ings, then the dielectric chamber becomes unnecessary. Thus,
the, entire heating system can be located within a heated me-
tallic casing. Besides assuring sufficiently good vacuum con-
ditions, in such a case it is possible to ensure a high degree of
electrical safety for the high-frequency heating circuit and,
consequently, to have the possibility of increasing the power
supplied to the plasma.
The considerations presented above will serve as subjects
for investigation in future experiments. In this paper, only the
first experiments on the observation of ion cyclotron resonance
in plasma bunches are described.
The experimental equipment is schematically shown in
Fig. la. The magnetic field is created by a solenoid during the
time a condenser bank is discharged through it. The topography
of the magnetic field is shown in Fig. 1b. There is a uniform
portion 50 cm long where the nonuniformity does not exceed
116; there are two magnetic beaches and a plug at the system
exit. The half-life of the magnetic field is 20 msec. High-
frequency power is introduced into the plasma by means of the
heating coil which is an inductance in the high-frequency cir-
3,2 4,8 6,5 8,1 cuit and which has a wave length Xz= 20 cm. The high-fre-
H, kG
Fig. 3. High-frequency circuit voltage as a
function of magnetic field intensity.
quency circuit, designed for a frequency of 10 Mc, is supplied
from a generator with a power of 100' kW. The plasma tube,
located along the solenoid axis, is in the form of a molybdenum
glass tube 75 mm in diameter and 2 m long. A vacuum of the
order 10-6 mm Hg is maintained in the tube. Plasma bunches
are injected into it from an electrodeless plasma gun. The gun is located at a distance of 45 cm from the edge of
the uniform portion of the magnetic field and in a region where the magnetic field intensity is close to zero. Ad-
mission of the gas is accomplished by a pulsed valve (not shown in Fig. 1). The working gas is hydrogen which
passes into the valve through a palladium filter.
The timing of all the elements of the equipment was so chosen that the bunches reached the heating coil at
the time of maximum intensity of the longitudinal magnetic field.
In the experiments, the velocity of the bunches which moved along the longitudinal magnetic field and the
dependence of the high-frequency circuit voltage on magnetic field intensity were measured.
The bunch velocity, Vz, was measured with an electrical probe, placed in the plasma; it was measured by
means of photomultipliers, and it was also evaluated from the rise rate of the loading introduced into the high-fre-
quency circuit by the bunches.. All these methods gave approximately the same result: Vz a 6.106 cm/sec.
The shape of the loading introduced into the high-frequency circuit by a bunch is shown in the oscillogram
in Fig. 2 for the case where the magnetic field intensity was less than the cyclotron value. Here, the straight line
indicates the base line, the point at the top-the magnitude of the voltage in the circuit prior to the appearance of
a bunch within the heating coil. The loading has a rise time approximately 6 psec long. Considering that the load-
ing rise time is equal to the time during which the bunch fills the entire heating coil, one can evaluate the bunch
velocity in the magnetic field. It was equal to ^-7. 106 cm/sec. From the curve in Fig. 3, one can make some
judgement about bunch loading of the high-frequency circuit as a function of magnetic field intensity. There is a
certain optimal region of magnetic field intensity values from 1.0 to 2.5 kG where the loading is maximal.
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10 I
I I
Vei Mr om ih2
5,95 6,1 6,25 6,4 6,55 6,7 685 7,0 7,15 7,3 7,45 7,6 7,75
H, kG
Fig. 4. High-frequency circuit voltage as a function
of magnetic field intensity (two magnetic beaches).
Fig. 5. Resonance loading for two different portions
of a bunch depending on the generation of waves with
frequency wt (one magnetic beach).
For weak fields, the loading is small because of
low bunch density on account of particle loss at the tube
walls. With increasing fields, the loading increases and
reaches a maximum for the value H =1.6 kG. With fur-
ther increase in the field, it falls; this probably occurs
both because of the reduction in bunch radius with con-
sequent weakening of its coupling with the heating coil
and because of reduction in bunch density resulting from
particle reflection at the entrance to the longitudinal
magnetic field.
After protracted break-in of the chamber by high-
frequency discharge, the measurements that were made
indicated the presence of two absorption peaks (Fig. 4)
symmetrically located with respect to some value Hm,
and the existence of a large value Hci corresponding to
ion cyclotron resonance for individual ions. The shift
of the high-frequency power absorption peak from Hci
in the direction of larger magnetic fields is evidence of
power consumption by the generation of ion cyclotron
waves [4]. One can determine plasma density from the
magnitude of this shift. With our experimental condi-
tions, the cyclotron absorption of high-frequency power
was small in comparison with nonresonance absorption,
obviously because of the weakening of the coupling be-
tween plasma and high-frequency circuit at higher values
of the magnetic field. Such a dependence was repeated
from experiment to experiment, and the curve in Fig. 4
is typical.
The existence of two absorption peaks can be explained by a Doppler shift in the frequency of the generated
ion cyclotron waves which are propagated in both directions from the heating coil-along the moving bunch and in
the opposite direction. These two frequencies should equal, respectively
c,ti=coo-k1VZ.and toy=wo -Ir- kzVZ,
where wo is the resonant frequency of the circuit; kz= is the component of the wave vector directed along the
z
axis; Xz is the excitation wave length, equal to the wave length of the heating coil.
Having the experimental value Aw= w2-wt, one can determine the bunch velocity averaged over the length
of the heating coil.
For the bunch velocity, we have the formula
C./'2 e/'/1 \
V_ _ McMc
which is obtained from the equality Aw = w2- wt with consideration being given to the dispersion relation for ion
cyclotron waves [4]. Here, Hl and H2 are the magnetic field intensities for which cyclotron waves are generated
with frequencies wt and w2, respectively; Hci is the magnetic field intensity for which the resonance condition for
individual hydrogen ions in a stationary plasma is fulfilled; Hm is the value of the magnetic field intensity for which
cyclotron waves are generated in a stationary plasma; e, M, c, are, respectively, ion charge, ion mass, and the vel-
ocity of light. For the values of Hl, H2, Hci, and Hm shown in Fig. 4, the bunch velocity Vz equals -6.7 ? 106
cm/sec. This is in agreement with bunch velocity measurements by other methods.
The bunch density, ni, averaged over the length of the heating coil was calculated from the dispersion rela-
tion for a stationary plasma [4]
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ni 11I,, 1
III/Id i? 10-17 Xz
and was -7' 1012 cm-3. Note that probing a bunch with an 8 mm microwave signal indicated the existence of a
plasma with a density not less than 1.6. 1013 cm-3 under these conditions. It appears reasonable that bunch param-
eters change with time; therefore, all comparisons of plasma parameters must be carried out for a fixed instant.
The curves shown in Fig. 5 represent the same functional dependence as in Fig. 4 but for the case where there
is no beach at the point where the bunch enters the uniform magnetic field. As can be seen from the curves, ab-
sorption of high-frequency power at the frequency w2 is not observed.
In Fig. 5, resonance loading is shown for two different regions of a bunch which are -1 m apart. Curves 1 and
2 correspond to two oscillogram traces. The time interval between them is -20 psec. The relative shift of the res-
onance peaks with the field arises, obviously, from a differenence in the velocities in the selected regions of the
bunch. In this case, the difference amounts to -21o. The curves shown illustrate the fact that regions more removed
from the forward boundary of a bunch move at lower speeds.
Thus, absorption of high-frequency power was experimentally observed for plasma bunches at two frequencies,
shifted by the Doppler effect in both directions from some mean frequency which, in its turn, was shifted toward
lower frequencies with respect to the cyclotron frequency for individual hydrogen ions. Such a shift corresponds to
the generation of ion cyclotron waves.
Magnetic beaches play an important role in the damping of these waves. With two beaches (at both ends of
the heating coil), waves with frequencies wl and w2 can both be damped, and therefore two high-frequency power
absorption peaks are observed. If a steep nonuniformity in the magnetic field replaces one of the beaches, then a
wave would be reflected at that point and would return to the coil region. In such a situation, the second absorption
peak should not be observed. This was verified experimentally.
Measurements of the amount of Doppler shift make it possible to fix the average velocity of a bunch. Deter-
mining Hci and Hm, it is possible to obtain information about plasma density. It is obvious that, by getting the time
dependence of the quantities mentioned, one can also determine the velocity and density distribution in the plasma
along the length of a bunch.
The authors express their deepest gratitude to K. D. Sinel'nikov for discussions of the results.
LITERATURE CITED
1. K. D. Sinel'nikov, et al., Zh. tekhn. fiz., 30, 282 (1960).
2. W. Hooke, et al., Phys. of Fluids, 4, 1131 (1961).
3. N. I. Nazarov, et al., Zh. tekhn. fiz., 32, 536 (1962).
4. T. Stix and R. Palladino, Phys. of Fluids, 3, 641 (1960).
All abbreviations of periodicals in the above bibliography are letter-by-letter transliter-
ations of the abbreviations as given in the original Russian journal. Some or all of this peri-
odical literature may well be available in English translation. A complete list of the cover-to.
cover English translations appears at the back of this issue.
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IN THE TERNARY FISSION OF U235
V. N. Dmitriev, K. A. Petrzhak, and Yu. F. Romanov
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 6-11, July, 1963
Original article submitted August 23, 1962
We measured the energy distributions of ternary fission fragments corresponding to different energy
intervals in the spectrum of long-range alpha particles with average energies of 10.6, 16.4, 20.3,
and 24.0 MeV. It was found that for Ea> 15 MeV the most probable total energy of ternary fission
fragments, within the limits of experimental error, was independent of the energy of the alpha par-
ticles and that for E. =10.6 MeV it was about 4 MeV higher.
The results of the measurements are evaluated.
Experimental data on the relation between the kinetic energy of fragments and the energy of long-range alpha
particles in the ternary fission of nuclei are of great interest. They are necessary for estimating the degree of de-
formation of the nucleus when ternary fission takes place and for formulating a hypothesis concerning the mechan-
ism of ternary fission.
Earlier measurements [1], in which we recorded alpha particles over a fairly wide energy range (from 13 to 22
MeV), showed that for Uzs5 the difference between the most probable total kinetic energies of fragments from binary
and ternary fission was 15 MeV. It is quite natural that the most probable ternary-fission fragments should be com-
pared with the most probable alpha particles, whose energy, as is known, is 15 MeV. From this it was deduced that
rbitt- Eterr& Ea? (1)
On the basis of the previously discovered fact [2] that the average number of neutrons in ternary fission is in-
dependent of the energy of the long-range alpha particles, it was assumed that Eq. (1) is valid for less probable fis-
sion conditions as well. This assumption was not contradicted by any other experimental data on ternary fission.
In order to verify Eq. (1), in the present study we measured the energies of paired U235 fragments corresponding
to separate energy intervals in the spectrum of long-range alpha particles. The experiments were conducted on the
reactor of The Leningrad Institute of Physics and Technology of the Academy of Sciences, USSR.
The Selection of Energy Intervals in the Spectrum of Long-Range A lpha Particles
The ternary ionization chamber and the electronic equipment used in the study were described in [1, 3]. An
important change in the design of the alpha particle recording chamber was the introduction of a shielding grid (Fig.
1), which ensured that the magnitude of the pulse was independent of the angle of incidence of the alpha particle;
the signal-to-noise ratio was increased, and the working volume of the chamber was limited. When the grid was
introduced, the experiments were conducted at intense neutron fluxes of the order of 5. 108 neutrons/cm2 ? sec. The
grid consisted of two coaxial rings encircling the collecting electrode and having diameters of 120 and 180 mm; a
tungsten wire 0.1 mm in diameter was wound radially around the rings. The inner ring was 8 mm high, the outer
ring 12 mm. Fluoroplast uprights were used to attach the entire structure to the annular collector. The chamber
was filled with argon (95%) and methane (5%) to a pressure of 1 atmosphere. The addition of methane ensured a
constant pulse front ('1 psec) and a stable pulse amplitude (over a period of 10-15 days the amplitude did not vary
by more than 2%).
Alpha particles with energies in a fixed interval were isolated by means of pieces of aluminum foil separating
the volume of the alpha chamber from the volumes of the fission chambers. Since the latter were of finite dimen-
sions, an alpha particle was braked both in the foil and in the volume of the fission chambers. The amplitude of the
pulse in the alpha chamber is maximum in the case when the end of the path of an alpha particle coincides with
the boundary of the working volume of the alpha chamber. By using an amplitude discriminator it is possible to re-
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Fig. 1. Schematic diagram of the electrodes of
the ternary ionization chamber: 1) fission cham-
ber collector; 2) fission chamber grid;. 3) conical
electrode of alpha particle recording chamber; 4)
aluminum foil; 5) alpha chamber grid; 6) alpha
chamber collector; 7) common electrode of fis-
sion chamber; 8) target.
as well as the necessary discrimination threshold.
. intervals, and
cord the alpha particles whose pulse amplitudes are greater
than a fixed value A1. Pulses with amplitudes between Amax
and Al will correspond to alpha particles whose initial energy
lies between Et and E2. Thus, the selection of an energy inter-
val in the spectrum of long-range alpha particles reduces to
the choice of the appropriate thickness of aluminum foil and
the choice of a specific discrimination threshold in the alpha
channel.
To determine the necessary discrimination threshold one
must know the working volume of the alpha chamber. This
was found by measuring the spectra of natural alpha particles
from U233 at reduced gas pressure; a U233 source with high alpha
activity was put in the place of the U235 source. By comparing
the calculated values with the experimentally determined varia-
tion of pulse amplitude as a function of gas pressure, we found
that the effective working volume of the alpha chamber was
between rt = 6 cm and r2 = 8.5 cm. We calculated the ampli-
tude distribution of the pulses from long-range particles at a
gas pressure of 1 atmosphere and varying thicknesses of foil,
Table 1 shows the thicknesses of the foils used, the selected energy
the average energies of the alpha particles, obtained from a known energy distribution [4].
TABLE 1. Average Energies (E) of the Selected Groups TABLE 2. Number of Recorded Ternary Fissions
of Alpha Particles
Foil thickness,
-
mg/cm2 Et-E2, MeV
E, MeV
-
9-12
10,6
21
15-18
16,4
36
19-22
20,3
51
23-26
24,0
Foil thick-
Ntern/Nbini
nterm
ntcrn,
ness;
mg/cm2
N
tern
x 640.0
exper.
calc.
-
6400
0,36
0,78
0,80
21
4300
0,46
1,00
1,00
36
4400
0,24
0,52
0,51
51
3400
0,096
0,19
0,15
The resolving power of the alpha chamber was determined chiefly by the finite dimensions of the source. At
.a pressure of 29 cm Hg the half-width of the line from the natural U233 alpha particles was about 2516. If we take
account of the fact that 1.6 MeV was released in the working volume of the chamber, we may assume that the en-
ergy of an alpha particle can be measured to within 0.2 MeV at a pressure of 29 cm Hg and about 0.5 MeV at 1 at-
mosphere. These accuracies for the measurement of long-range alpha particle, energies were sufficient, since no
energy intervals narrower than 4 MeV could be distinguished under the experimental conditions. These conditions
relate primarily to the "single-channel" nature of the experiment, the comparatively small solid angle of the alpha
chamber with respect to the target (about8To), and the low probability of production of alpha particles with energies
greater and less than 15 MeV.
Results of the Measurements
In the experiments we used U235 targets with thicknesses ranging up to 20 pg/cm2 and an area of 1.5 cm2. The
backing for the target was an organic plate with a thickness of 5 pg/cm2 and coated on both sides with gold layers
having a combined thickness of 10 pg/cm2. The number of binary fissions reached values up to 120,000 per minute.
Table 2 shows the number of ternary fissions recorded for each of four alpha particle energy intervals, the ratio
of the number Ntern of ternary fissions to the number Nbin of binary fissions, the relative count values ntern and the
relative probability of finding an alpha particle in a given interval, as obtained from the energy spectrum of long-
range alpha particles [4].
The agreement between the experimental and calculated values of ntem indicates that the selected energy
intervals in the spectrum of long-range alpha particles were correctly determined. For the interval with an average
energy of 24 MeV we obtained a somewhat high count value, which may be explained by the following: it is known
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[5] that for alpha. particles with energies of more than 20 MeV the angular distributions of the fragment divergence
lines is nearly isotropic. Under the conditions of the experiment described above, alpha particles with an isotropic
angular distribution are recorded with a higher probability than alpha particles which have the characteristic aniso-
tropic distribution with a maximum near 90?. In view of this the count value for a. foil thickness of 51 mg/cm2 is
less surprising.
40 50 60
Number of channel
N( tern
56,3
300
, T
36,4
T
i f
53,54
r
Zoo
3
jf r
10
Ntern
50
32,8
1
0
36
100
f t
1
7 t
1o
1
s
o
t
1,
i
0
40 s0 60
Number of channel
b
Fig. 2. "Two-humped" energy distribution of binary-fission fragments Nbin (---) and ternary-fission
fragments Ntern (-): a) E? = 10.6 MeV; b) Ea = 24.0 MeV.
Ntern
500
92,8 98
,t
250
i
t 10%
LA
`
90 100 110
Number of channel
a
~0
90 100 110 f?D
120
Number of channel
Fig. 3. Number of fissions as a function of the total kinetic energy of the fragments (a and b are the
same as in Fig. 2).
Ntern
200
0 10
100
o
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To measure the energies of the ternary fission fragments we used both a multichannel amplitude analyzer and
a special cathode-ray tube analyzer with a photographic attachment [1, 3]. The energy shifts of the peaks in the
"two-humped" distributions of binary and ternary fission fragments were found by means of a multichannel analyzer.
As an illustration, Figs. 2a and 2b show the results of one of the series of measurements. In case b we use a thicker
target, which produced a reduction in the pulse amplitudes and in the peak-to-trough ratios. This fact is of no great
importance, since the measurements are relative. In Figs. 3a and 3b, for the same series of measurements, we show
the variation of the number of fissions as a function of the total kinetic energy of the fragments, as obtained from
an analysis of the photographic plates. The values of the chosen channels in both cases are arbitrary and are not
equal to the analyzer channel value; this is due to the different magnification of the projector.
Table 3 shows the differences between the energies of the most probable light and heavy binary and ternary
fission fragments, Ml and Mh.
TABLE 3. Differences Between the Energies of Light and Heavy
Fragments Produced by Binary and Ternary Fission
Ea, MeV
DEl,MeV
~"Eh, MeV
AEl + ~Eh, Me
10,6
6,0 ? 0,6
4,9 ? 0,6
10,9 ?1,2
16,4
20,3
8,5 ? 0,6
9,3 ? 0,8
6,5:1- 0,6
5,5 ? 0,8
15,0 ? 1,2
14,8 ? 1,6
24,0
9,6 ? 0,8
5,9 ? 0,8
15,5 ? 1,6
Ntern
1
S00
i?
'
M
T
i
:
\
I
1
2,0 E, /E7
b
Fig. 4. Number of fissions as a function of fragment energy ratio (a and b are the same as in Fig. 2).
The tabulated data include corrections for ionization caused by the alpha particles in the fission chambers.
The last column of the table shows the total energy difference, Ml + Mh. It can be seen from the. table that if
Ea > 16 MeV, the difference between the energies of binary and ternary fission fragments remains constant, within
the limits of experimental error. This means that in ternary fission the total kinetic energy increases as the energy
of long-range alpha particles increases and that it may considerably exceed the total energy of the most probable
binary fission fragments.
By processing the data corresponding to each alpha particle energy interval, we obtain graphs of the number
of ternary fissions as a function of the fragment energy ratio Et/E2 (Et/E2 ^' M2/M1). The resulting relationships show
that in all cases the mass distributions of ternary fission fragments for different energies of long-range alpha particles
1,I4
Ntern 1
200
100
0
?
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are approximately equal, and the maximum values of the distributions are found for the same mass ratio, about 1.5
(Figs. 4a, b). The difference between the peak-to-trough ratios may be explained by the thickness of the targets
used, and the relatively small trough in each case is caused by the absence of a collimator, which could not be used
in principle under the conditions of the experiments.
Evaluation of Results
The experimental data obtained in the present study indicate that as the alpha particle energy increases from
10.6 MeV to 16.4 MeV, the most probable total kinetic energy of the fragments is reduced by about 4 MeV. This
means that Eq. (1) apparently applies only in the region of low alpha particle energies (up to 15 MeV). The energy
shifts of the most probable ternary fission fragments in comparison to those of the binary fission fragments indicate
that the effect of distance between the fragments at the moment of fission depends on the energy of the alpha par-
ticles if Ea < 15 MeV but is independent of it if Ea> 15 MeV. It may be assumed, therefore, that the mechanisms
of alpha particle emission in these two regions are different.
From the increase in the total kinetic energy of the fragments and alpha particles as the alpha particle energy
increases for Ea > 15 MeV we conclude that the internal excitation energy of ternary fission fragments decreases for
high values of Ea.
From the similarity of the mass distributions of ternary fission fragments for different alpha particle energies
it follows that for each chosen interval of mass ratios the energy spectrum of long-range alpha particles must be
approximately the same (1.1 < Ml/M2< 1.8).
LITERATURE CITED
1. V. N. Dmitriev, et al., Zh. eksperim. i teor. fiz., 39, 556 (1960).
2. V. F. Apalin, et al., Atomnaya energiya, 7, 375 (1959).
3. V. N. Dmitriev, et al., Pribory i tekhnika d'ksperimenta, No. 1, 94 (1962).
4. C. Fulmer and B. Cohen, Phys. Rev., 108, 370 (1957).
5. N. A. Perifilov and Z. I. Solov'eva, Zh. eksperim. i teor. fiz., 37, 1157 (1959).
All abbreviations of periodicals in the above bibliography are letter-by-letter transliter-
ations of the abbreviations as given in the original Russian journal. Some or all of this peri-
odical literature may well be available in English translation. A complete list of the cover-to-
cover English translations appears at the back of this issue.
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DISTRIBUTION OF THE NUMBER OF COUNTS ON A NEUTRON DETECTOR
PLACED IN A REACTOR
V. G. Zolotukhin and A. I. Mogil'ner
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 11-16, July, 1963
Original article submitted July 18, 1962
A discussion is given in the stochastic process of neutron multiplication and detection in a nuclear re-
actor. The use of physically justifiable assumptions makes it possible to simplify the mathematically
complicated problem and find the productive probability function for the number of counts in a def-
inite interval of time. The distribution found has been confirmed experimentally. Some applications
of the theory are indicated for determining the reactor kinetic parameters.
The interest in the theory of reactor noise, due mainly to new experimental possibilities of determining re-
actor parameters, has stimulated the appearance of a number of theoretical and experimental papers. In the gen-
eral case, equations are written for the mean values and fluctuations of the neutron density [1], and on the assump-
tion of elementary nuclear reactor theory, expressions have been found for the autocorrelation function of the de-
tector counting rate [2], the dispersion of the number of counts [3-5], and the fluctuation in the total number of neu-
trons in the reactor [6].
In [7), the question is posed of the distribution. of the number of neutron detector counts in a definite interval
of time. It turned out, as in the theory of cascade processes, that the Polya distribution provides a certain approxi-
mation to the exact distribution, but is in some respects unsatisfactory.
Knowing the distribution of the number of detector counts is also of practical importance. The statistical
methods used at the present time for investigating the kinetic parameters of subcritical reactors, employing the data
of a discrete neutron detector, are based on making an experimental determination of the autocorrelation function
of the counting rate (Rossi-alpha method) or of the dispersion in the number of counts (Feinman-alpha method). This
requires a rather long time for practical measurements, or complicated apparatus for accumulating sufficient in-
formation to achieve the required accuracy in the parameters being determined.
In contrast with the above methods, the probability method, the basic ideas of which have been presented in
previous papers by the authors [7, 8], is based on knowing the probability distribution law for the number of neutron
detector counts. Knowing this law makes possible a great reduction in the time required to accumulate the data.
Further, the probability method makes it possible to use relatively simple apparatus, combined with automatic treat-
ment of the information for intervals of different lengths.
This paper gives expressions for the probability Pk(t) of having k detector counts in the time t. This distri-
bution depends on two kinetic parameters of the reactor, which may be found by comparing the distribution found
experimentally with the theoretical distribution. The productive function is also found for the distribution of the
number of counts in two nonintersecting time intervals, which makes it possible to treat the experimental data. The
distribution Pk(t) is confirmed experimentally, and a description is given of some of the possible applications of one
of the forms of the probability method.
Choice of Model and Solution of Equations for the Productive Functions
It is assumed in the discussion that the reactor is subcritical, and that the steady state power level is main-
tained by an external neutron source of strength S neutrons/sec, with a Poisson distribution of the emitted neutrons.
Three elementary factors tending to change the number of neutrons in the reactor are important in describing
a microscopic reactor model: 1) neutron loss resulting from leakage and pure absorption; 2) counting loss; and 3)
fission, with generation of new neutrons. In these processes, an exponential distribution law is assumed forthe partial
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lifetimes, with the time independent constants, Xc, Xp, and X f , respectively. The probabilities Pr, f that fission of
a fuel nucleus will give u secondary neutrons are known [9]. In the present model, the effect of delayed neutrons
is neglected, which is permissible for a detection time much less than the mean lifetime of the delayed neutrons.
Since interactions between neutrons and matter and their detection under small loadings are clearly defined
discrete events, it is convenient to use the productive probability function apparatus (abbreviated p.p.f.).
We introduce the following p.p.f.:
1. H (x) is the p.p.f. of the number of neutrons in the reactor at an arbitrarily chosen instant of.time (in the
steady state case).
2. F1 (x1, x2, t) is the p.p.f. of the number of neutrons in the reactor at the instant of time t, and of the num-
ber of neutrons detected in the time t, under the condition that there was one neutron in the reactor at the instant
of time t= 0.
3. P(x, t)=F1(1, x, t) is the p.p.f. of the number of neutrons detected in time t, owing their origin to the neu-
tron that was present in the reactor at t = 0.
4. llt(x) is the p.p.f. of the number of neutrons detected in the time t.
Making use of the familiar properties of the p.p.f. and the Poisson distribution, it is not difficult to obtain the
following relations:
H (x) _= exp (S S IF1(x, 1, T)-11 dt)
0
I
lll(x)=II(11 (x, t))ex1) S`~ P(x,T)-11dt).
To find the p.p.f. F1(x1, x2, t), we make use of the theory of random branching processes developed by A. N.
Kolmogorov and N. A. Dmitriev in [10]. This considers n types of particles, T1, T2, ..., Tn, with possible conver-
sions of one into the other. The state of the system is given by the n-dimensional vector a, with the integral com-
ponents al, a2, ..., an, equal to the number of particles of each type. Let one particle of type Tk have the prob-
ability Pk(a, t1, t2) of being converted in the time (t1, t2) into the assembly characterized by the vector a. If the
probability Pk(a, ti, t1+ A) may be represented in the form
1Pk(a, ti, ti-;-A)=hu+A(a, t1)A-f-o(A),
k _ 1 11 if a; _ (), i * k, ak = 1;
I"j = 0 in all other cases;
. then, for the productive functions in the case of a homogeneous process
r/ Flt {
. I - (Fi, F21 ? ? , F,),
,)Fk 1 { JFk
tit J ;.T (xi, x2, .7 X11) - J:tj
j-l
with the initial conditions Fk(x, 0)= xk. In Eqs. (2), fk(x) is the p.p.f.; thus
Fk (xi, x2, ..., x, , t) = 1 ... x;atxt, ... xanP1 (a, t)
a1=0 as=0 rjn=0
, (x) = LJ L ... LJ ga (a1, C(2, .. (III ) xiixa2 ... , xa,,
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Assigning the neutrons present in the reactor to the particles of the first type, and the detected neutrons to the
particles of the second type, using the present model, we obtain
ft (x1, x2) = a c (i - xt) + X p (x2 - x1) +
+ ~f [y (x1) - x11;
f2(xi, x2) = 0,
where y (z) = I Ph, fzk is the p.p.f. of the number of prompt fission neutrons.
h=O
Noting that F2(x1, x2, t)= x2, we obtain for Ft(x1, x2, t)
ad'F1)+Xp(x2-F1)+),f[y(F1)-F1
and for P (x, t) = F1(1, x, t) and F (x, t) = F1 (x, 1, t)
aP P)+?p(x-P)+?f[y(P)-P1;
(with P(x, 0)=1 and F(x, 0)=x].
aF
H (x) =exp CS [F1 (x, 1, t) -1] di) = exp S (r-1) dr 1
) kc (1-r)+),p (1-r)-4-Xf [y (r)-r] % - (7)
0 x .
Further, from (1) and (7) we find
P(x, t)
1t1 IIt (x) = S (r-1) dr
(~c+~p) (1-r)+~p (x-1)?X f [y (r) -r]
+S (r-1)dr
(~c } gyp) (1-r)+~f (1-r)
P(x, t)
Taking ac+ X. = X, C, and differentiating in ITt (x) with respect to t, using (5) we find
a In 11t S [P (x, t)-1] Xp (1-x)
at ),;(1-P)-I-Xf[y(P)-P]
IIt(x)=exp(SXp(x-1
t
[1-P (x, t)] d-r
X ~ ?e[1-P(x, t)1+Xf[y(P)
0
P(x, 1)
dz
t -i-'%f)(1-z)+xP(x-1)+Xf[y(z)-z]
_ dz
t a 1-z-[ ap (x-1)+ of [y (z)-1-v (1-z)]
dy (z) 1-Kr
where V = dz is the mean number of secondary fission neutrons, a= t
o
is the fast neutron multiplication factor, and 10 is the mean neutron lifetime.
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Although the p.p.f. y(z) may, with good approximation, be taken in the form
Y (z) _ (1 I v (1 M -Z))m
'
where m = 5-7, the problem of making an explicit solution of (8) and (9) for llt(x) is exceedingly complicated. How-
ever, there is no need for using the exact form of the function y(z). Under actual conditions, the probability of de-
tecting one or more neutrons owing their origin to the one original neutron is exceedingly small as a result of the
smallness of the detecting efficiency. It is hence clear that the function P(x, t) is very close to unity for all values
0 < I x I < 1. Accordingly, in the expression under the integral sign in (9), we can limit ourselves to an expansion
of y(z) in Taylor's series keeping the first three terms, and then, after evaluating the integral in (9), and solving for
P(x, t), we obtain
P (x, t) = 1 - .1 - (q-1) (1-a-atD)
iA + T-1 a-at(p
v (v-1)
A= atf (P-Y1 ? 2z (1-x);
v(v-1)R
Tf= ~f ; R=? tf.
The quantity R is the detector efficiency for fission counts in the volume of the reactor. In the denominator
of the expression under the integral sign in (8), we can also limit ourselves to three terms of the expansion of P(x, t)
in Taylor's series, so that
Sk p (x-1) dt
In f1t (x) = -a 0 C1~ v(v 1) (1 P)J
l_ f
from which, using (10), after integrating and some rearrangements, we obtain l
In 11, (x) Z' { 1- (P - a x In [ 1+ (T, )2 (1- e-?tw) J (11)
where m is the mean number of counts in time t.
The distribution with p.p.f. (1) depends on the three parameters at, z, and m, and has the following central
moments:
62=m[1+zcP1(at*
R3 = rn 11 + 3zcpt (at) + 3z2cP2 (at)l;
?4 = 3a4 + m [1 + 7zcpt (at) + 18z2cP2 (at) +
+15z3cp3 (at)l,
X
cPz (x) +e-x 2 (1 - e-x)
S.
W3 (x) =1,- 3 (1-e-x) + 2e-x+
X
1 (1-e-x)2 4xe-x
+10 z + 10
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It may be shown that,as z- 0, the distribution of the number of counts reduces to the Poisson distribution.
The asymptotic expansion of the probabilities Pk as m --> 0 is of the form
2
e-x h/2
Pk /
.1 61 H3 (xk) + V2 24 Ha (xk) 172 H6 (xk) ] '
2 is L rr
19
Yt= 63
Y2= Ira 6q -3, xk =
and the Hk(x) are Hermite polynomials.
The quantity Q = 1 In Pot, equal, from (11) to
m
(tPo -1)2 vi(P o
1 - i ((Po -i) In 1 - f - ~ } t P o (1-e
Q (t) _ --ac -- -- 1, { To
where q0= 1 , may be used to find the parameters a and z, if there are measurements of Q for at least two in-
tervals t.
The exact distribution was compared with .the Polya distribution. For at it is a simple matter, from the
p.p.f. (11) to find the recursion relation for the probabilities:
k
M Pk+1 Pk_ (2/ -1)! I z i
(1-+-k) I+2z o j j! C1-1-2z
j
while the Polya distribution with the correct two moments gives
m -I- k s Po _ (1 + Z)-m/_
Figure 1 shows these distributions for m = 5, and z= 1. The difference between them is small, particularly for
small z.
By following the method presented above, we can find the p.p.f. of the number of counts in two nonintersect-
ing intervals of the same duration t, separated by the time interval T-
1-1 (x1, x.,, t, T) It (xi) Ilt (x,) `< expl. -- a Z In [1 - y (xt) Y (x2) e-"t 1 J
Y J. - y~ 1+(cp!}~)2
(1-P-?fw)
(here ~P (y) = J/1 ? 2z (1 - y)),
and fTt(x) is given by Eq. (11).
Experimental Check on the Distribution
The results obtained in the preceding section are based on an idealized one group and one zone nuclear re-
actor model. The question of how correctly this model reflects all the essential features of the multiplication proc-
ess in an actual physical reactor must be solved experimentally.
* The expression (12) which is a special case of the distribution (11), was obtained independently by L. P,11 [111,
whose work became known to the authors while they were preparing.the present paper for publication. The produc-
tion function (11) was found in 1960, and was awaiting experimental confirmation.
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Measuring the probability Po(t) of having no counts in the time t is a sensitive method of finding the param-
eter a, which is of the greatest interest.
An experimental check on the distribution consisted in comparing the values of the quantity a obtained by
the Po-method and by the independent method of C. Cohn [12]. The latter is based on a spectrum analysis of the
noise in the ionization chamber current which measures the neutron flux in the physical reactor, and is only asso-
ciated with a type of counting rate autocorrelation function confirmed by numerous experiments.
a, sec-t
Fig. 1. Distribution of the number of neutron de-
tector counts (histogram), and Polya distribution
(solid curve) for m=5, z=1, and at= -.
1500
100
FOO
'
1
I
-
Fig. 2. a =1 Kp as a function of the
I0
number LN of fuel channels removed.
The measurements were made on a thermal assembly, the active zone of which contained uranium enriched
to 9016 in the U235 isotope, with hydrogen moderator and a beryllium reflector. In finding the value of Po(t), use
was made of a six channel statistical analyzer employing transistor-ferrite elements, operating on the principle set
forth in [8]. In four minutes, each channel analyzed about 106 time intervals, which gave high statistical accuracy
in the results.
The neutron detector was a standard SNMO-5 proportional counter, filled with BF3 gas having enriched boron.
The detector was converted from proportional operation to an ionization chamber by lowering the voltage. In mak-
ing measurements by C. Cohn's a-method, the reactor power was increased by means of an external source. After
preliminary amplification, the noise in the detector current was passed through a resonance filter. The constant com-
ponent of the detected signal, taken from the circuit, was recorded on the chart of an automatic EPP-09 potentio-
meter. The spectrum analysis was made in the frequency range 26-125 cps.
The normalized value of the spectral density of the noise in the current is known to be of the form
w2 .f a2
with constant values of A and B (w is the angular frequency). The best value of at was obtained from a set of ex-
perimental values using the method of least squares.
In the Po-measurements, the six intervals tk were related by the equation tk = tl ? 2k-1, with ti = 0.32. 10-3 sec,
where k is the number of the interval for which the value of Po(tk) was measured. The values found for Q(tk) were
treated by the method of least squares on a BESM-2 computer. The result of the measurements by the Po-method was
a = (420 ? 20) sec-1 ,
and by the spectrum method
a = (400 ? 50) sec-1.
These values agree with one another within the limits of error shown.
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It is interesting to note that using the Pp-method for eight minutes gave an accuracy of 5% while the spec-
trum method (for eight frequency values) only gives an accuracy of 12% for 80 minutes.
Determination of Large Subcriticalities by the Probability Method
A description is given of one of the experiments where the Pp-method was used to measure large negative
reactivities in one of the highly enriched uranium-beryllium homogeneous assemblies with a beryllium reflector,
and an intermediate neutron spectrum.
The Po-method was used to measure the values of a as the outside fuel channels were successively removed
from the active zone. Here it was assumed that in the function Keff= f (N-Ncr), where N is the number of identi-
cal operating channels in the active zone and Ncr is the critical number, there is a linear initial portion obtained
by expanding the function in Taylor's series using the first two terms. The value of a is also related to the reac-
tivity p by the linear equation
where ao = S. It was accordingly to be expected that as the fuel channels were successively removed from a reac-
0
for that was close to critical, the initial portion of the curve a(ON), where ~N is the number of channels removed,
would be linear.
In making the Po-measurements, the apparatus was used which was spoken of in the previous section. The
SNMO-5 counter was set up in place of one of the blocks in the beryllium reflector, adjacent to the active zone.
"Priming" with the external neutron source was only used at very large subcriticalities to improve the statistics. A
preliminary (5% accurate) determination of a from the set of experimental values of Q(t)= 1 1
m(t) In po(t) was made
graphically [we have previously spoken of a set of Q(z, at) curves]. The values of a was made more accurate on a
B14SM-2 computer.
The resulting a(zN) curve shown in Fig. 2 shows that there is an initial linear portion. If it is borne in mind
that the effectiveness of one fuel channel on the edge is 2.3 (3, it may be concluded from the curve of Fig. 2 that
the linear portion extends to subcriticalities of -'10 B.
Thus, using the present method enables measurements to be made successfully of negative reactivities at
least to -10 B, so that in this range, the probability method competes successfully with the pulsed source method
[11], with the convenient difference that the apparatus is simpler.
In conclusion the authors express profound gratitude to A. I. Leipunskii and G. I. Marchuk for their interest
in the work, to V. A. Kuznetsov for useful discussions and aid, to V. V. Sapozhnikov, who made up the apparatus
and took part in the experiments, and to G.. P. Krivelev and A. S. Postovalov, who took part in the experiments.
LITERATURE CITED
1. L. P'1, Nuovo Cimento. Suppl., 7, 25 (1958).
2. C. Veles, Nucl. Sci. and Engng., 6, 414 (1959).
3. Scientific and Engineering Bases of Nuclear Power, Vol. 2, edited by K. Goodman [Russian translation], Mos-
cow, IL, p. 18 (1950).
4. Feynman, D. de Hoffman, and R. Serber, J. Nucl. Enging., 3, 64 (1956).
5. J. Bengston, et al., Paper No. 1783, presented by the USA at the Second International Conference on the Peace-
ful Uses of Atomic Energy [Russian translation]; Geneva (1958).
6. E. Courant and R. Wallase, Phys. Rev., 72, 1038 (1947).
7. V. G. Zolotukhin and A. I. Mogil'ner, Atomnaya Energiya, 10, 379 (1961).
8. A. I. Mogil'ner and V. G. Zolotukhin, ibid., 10, 377 (1961).
9. King and Simmons, Nucl. Sci. and Engng., 3, 595 (1958).
10. A. N. Kolmogorov and N. A. Dmitriev, Dokl. AN SSSR, 11, 7 (1947).
11. L. Pal, Statistical Theory of the Chain Reaction in Nuclear Reactors, Part III [in Russian], Budapest (1961).
12. C. Cohn, Nucl. Sci. and Engng., 5, 331 (1959).
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V. N. Avaev, G. A. Vasil'ev, A. P. Veselkin, Yu. A. Egorov,
Yu. V. Orlov, and Yu. V. Pankrat'ev
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 17-20, July, 1963
Original article submitted August 25, 1962
The relaxation lengthsof research reactor neutrons were measured in polyethylene. The findings are
in excellent accord with data computed theoretically using the method of moments. The relaxation
lengths are '-15% less than in the case of water.
The function of polyethylene in nuclear engineering is as a biological shielding material for neutron shielding
[1]. The principal advantage of polyethylene over rival hydrogen-bearing materials is the high density of hydrogen
nuclei (7.92. 1022 per cm3) combined with a relatively low specific weight (0.92 g/cm3). For example, for the dose
rate due to 0.33-18 MeV neutrons to be reduced by 10 thousand times, a polyethylene slab of -61 g/cm2 is required
[2], while the thickness of an equivalent layer of water would be -81 g/cm2.'" In this case, the savings in shielding
weight may top 30%.
Effective energy
Energy range in de-
Indicator
cutoff, MeV; reson-
termination. of indi-
Size of indicator, mm
ance energy, eV
cator activity, MeV
Intts (n, y)
1.44 eV
0.9-1.7
Flat-10 x 10 x 0.2
I' (n, y)
30 eV
0.28-0.78
Cylinder, d=8, h=40
PS' (n, p)
2.8 MeV
6
Cylinder, d = 8, h = 40
A171 (n, p)
4.7 MeV
0.41-0.95
Clyinder, d=8, h=50
A127 (n, a)
7 MeV
1.1-2.85
Clyinder, d=8, h=50
The physicomechanical and chemical properties of polyethylene have been extensively studied and reported
on the literature [3]; studies on radiation effects on the properties of polyethylene are continuing. In particular, it
has been found that preirradiated polyethylene (up to 15-20 Mrad exposures), known under the name irrathene,
is stable at temperatures as high as 250?C, and its strength at 110?C is triple that of conventional unirradiated poly-
ethylene at the same temperature [4].
The shielding properties of polyethylene have been investigated by Broder, et al. [5] for neutrons o 4 and 14.9
MeV energy. Goldstein [2] has drawn inferences from findings of studies of the passage of neutrons through poly-
ethylene [2]. However, the amount of experimental data in the literature on the attenuation of pile neutrons by
polyethylene is still meager.
Experimental Geometry and Conditions
The experiments were carried out in a water-cooled water-moderated research reactor. A polyethylene prism
(680 x 680 x 1000 mm3) was placed in a recess formed in the heavy concrete reactor shield. The prism was made
up of square plates 10 and 20 mm thick.
Resonance indicators (indium, iodine) and a BF3-filled counter were used in the measurements of the distri-
butions of thermal and epithermal neutrons. The spatial distribution of fast neutrons was measured with the thres-
hold indicators P (n, p), Al (n, p), Al (n, a), and a bantam-size ZnS (Ag) scintillation counter. To avoid activation
of the threshold and resonance indicators by thermal neutrons, the indicators were sheared in 1 mm thick cadmium
jackets. The characteristics of the indicators employed appear in Table 1.
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2
100
6
Thickness of polyethylene slab, g/cmz
Fig. 1. Fast neutron distribution in polyethylene.
Computed data: 1) En> 7 MeV; 2) En> 4.7 MeV;
3) En>> 2.8 MeV. Empirical data: A) Al (n, p);
0) Al (n, a); ^) P (n, p); ^) ZnS(Ag).
In the course of the measurements, flat indicators were
lodged in the spaces between the platelets, and the round
cylindrical ones were placed in notches (20 x 20 x 100 mm) in
the plates. Four indicators were irradiated at a time, and mu-
tual shielding was averted by shifting them around the axis of
the prism at f 5 cm spacings.
The activity of the flat indicators was measured using a
27r -scintillation counter, and the activity of the cylindrical
ones was measured using a 4ir -scintillation counter. The coun-
ters were incorporated into the circuitry of a spectrometer in
order to reduce background and impurity effects in the indi-
cators, and instead of the integrated number of pulses, thenum-
ber of pulses due to the y-line or group of y-lines most char-
acteristic of the given indicator was recorded (see Table 1).
The spatial neutron distribution in polyethylene was
measured with a ZnS(Ag) scintillation counter (d> 20 cm
polyethylene thickness) and a BFs-loaded counter (at d> 30
cm). A slit 30 x 30 x 350 mm was cut in one plate to accom-
modate the counters, and this slit was moved around the prism
during the experiment. Measurements were carried out at each
point at several different reactor power levels in order to check
the counter sensitivity to y-radiation and in order to ensure
more reliable results.
Attenuation of Fast Flux
The measured distributions of fast flux (Fig. 1) were com-
pared with the results of a computation of distributions by the
method of moments for a point isotropic neutron source with a
fission spectrum [2]. The computed differential neutron spectra
were integrated according to the formula
18 MeV
N (d) _ ~ a (F) ? 9t (F, d) dE,
En
where o(E) is the cross section of the reaction [6] for an indicator of threshold En extrapolated to 18 MeV; 4)(E, d)
is the differential numerical neutron spectrum in polyethylene at thickness d; N(d) is the flux of neutrons with en-
ergies ranging from En to 18 MeV at thickness d.
TABLE 2. Relaxation Lengths of Fast Neutrons in Polyethylene (cm)
Thick-
ness of
ppof
eth
-
n
E > 7 MeV
E > 4,7 MeV
n
En> 2,8 MeV
Zns(Ag)
dose
y
yy
lnn2sla
Exper.
Theor.
i
Exper. Theor.
Exper.
Theor.
Exper.
Theor.
0-30
30-60
7,8
9,7
9,1
7,8
9,7 8 9
7,
8
8
6,6
8
2
7,5
-
7,1
60-90
-
10,7 9,5
,
9,5
,
-
8,2
,8.
8,8
g
,5
9,5
7,4
8,6
Clearly, in the light of Fig. 1, the experimental data points* obtained in measurements of the neutron flux
distribution with the indicator Al (n, p), i.e., in measuring the distribution of neutrons of energy greater than 4.7
* The experimental findings reported here take into account geometrical attenuation of neutron flux along the prism.
The correction for geometric attenuation was determined experimentally.
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106
8
4
2
S
10
9
10?
0
Thickness of polyethylene layer, g/cm2
Fig. 2. Distribution of thermal and epithermal neu-
trons in polyethylene: 0) In; zl) I; ,El) BF3 counter;
+) cadmium ratio, from results of In measurements;
x) cadmium ratio, from results of BF3 counter
measurements.
MeV, fit well on.the predicted curve. The results ob-
tained for neutrons of energy greater than 2.8 MeV [in-
dicator P (n, p)] also show a good fit, within the limits of
experimental error, with the theoretically predicted data
(with the exception of the first two data points).
For neutrons of energy greater than 7 MeV [indicator
Al (n, d)], the agreement between experiment and calcu-
lations is observed at a thickness greater than 30 g/cm2.
At lesser polyethylene thicknesses, sharper attenuation than
that anticipated in the calculations is observed (curve 1).
TABLE 3. Relaxation Lengths (cm) of Neutrons in Poly-
ethylene and in Water (Density of Polyethylene 0.92g/cm3,
of water 1 g/cm3)
E 4,7 MeV E,, 2,8 MeV
__.
..... .....
'Poly- ~Poly-
Water ~
Iethylene I ethylene l11
Water
TABLE 4. Relaxation Lengths (cm) of Thermal and Epi-
thermal Neutrons in Polyethylene and in Water
Layer thick-
Polyethylene
Hess, cm
Thermal- Water
1.44 nnr1311eV
1 ..- F
0-30
5,5
30-60
(i,9
6,8
60-90
8,8
9,0 8, 5
The neutron distributions measured with a scintilla-
tion counter and with the indicator P (n, p) are superposed
at 26 g/cm2 slab thickness, and agree within the limits of
experimental error.
In Table 2, relaxation lengths determined empirically and read off theoretically predicted curves are com-
pared. The excellent fit between theoretically predicted data and empirical data for all the energies at a poly-
ethylene thickness greater than 30 cm is quite conspicuous, and a substantial divergence is observed at lesser thick-
nesses in the case of neutrons of energy E> 7 MeV and E> 2.8 MeV. The discrepancies are apparently accountable
to some difference in the assumed and the actual spectra of the neutron sources [7] and the geometry (in reference
[2], calculations were carried out for a point isotropic source in an "infinite" medium, while the experiment involved
a plane source in a "semiinfinite" medium).
Table 2 also lists relaxation lengths for neutron dose rates Xdose calculated from the data reported in [2]. A
comparison of Xdose and the relaxation lengths for the neutron fluxes clearly reveals that the contribution of neu-
trons of energies 1-2 MeV to the dose is quite appreciable even at relatively large distances from the source.
In Table 3, relaxation lengths of neutrons in polyethylene and in water, measured under identical conditions,
are compared. The relaxation lengths in polyethylene are 12 to 17% less than the relaxation lengths in water.
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-
-
2
6
f0f
2
:
i
i
i
i
i
2
Y
'
4
v
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Attenuation of Slow Flux
The results of measurements of the spatial distributions of fluxes of neutrons, 1.44 eV (indium) and 30 eV
(iodine), are shown in Fig. 2. At close distances from the reactor core, the attenuation curves appear to have a
steeper slope than at great distances. The more abrupt attenuation experienced in the first polyethylene layers is
due to the absorption of neutrons slowed down in the core and in the water reflector of the reactor. The relaxation
lengths computed from the experimental results are given in Table 4, while the geometrical attenuation of the flux
is subject to the same correction as that applying to fast neutrons.
The curve describing the thermal flux distribution (see Fig. 2) at polyethylene layer thickness less than 50
g/cm2 has a gentler slope than the distributions measured by indium and iodine indicators. This is apparently ex-
plained by the leakage of scattered neutrons from the concrete shielding from the side of the unshielded end of the
BF3 gas counter.* At a large polyethylene thickness, satisfactory agreement is observed in the attenuation of ther-
mal and epithermal flux.
The cadmium ratios calculated on the basis of the results of our measurements (see Fig. 2) reveal that the
equilibrium spectrum of thermal and epithermal neutrons in polyethylene is established at layer thickness 20 to 30
g/cm2.
Table 4 offers, for comparison, relaxation lengths for water, as calculated form the data in reference [8].
The authors take this opportunity to express their gratitude to the staff working on the research reactor and to
the laboratory technicians who took part in the experiments.
1. Mod. Plastics, No. 10, 97 (1961).
2. H. Goldstein, Fundamental aspects of reactor shielding, Addison Wesley, USA (1959).
3. V. Shifrina and N. Samosatskii, High-pressure polyethylene, Moscow, State Chemical Press [in Russian] (1958).
4. R. Ward, Nucleonics, 19, No. 8 (1961).
5. D. L. Broder, A. A. Kutuzov, and V. V. Levin, Inzhener.-fiz. zhur., 5, 47 (1962).
6. D. Hughes, Neutron Cross Sections, BNL-Upton-New York (1958).
7. V. N. Avaev, et al., JAE, 15, 20 (1963).
8. K. Cooper, D. Johns, and K. Horton, Article in symposium "Shielding of nuclear-propelled vehicles" [Rus-
sian translation], Moscow, Foreign Literature Press (1961).
All abbreviations of periodicals in the above bibliography are letter-by-letter transliter-
ations of the abbreviations as given in the original Russian journal. Some or all of this peri-
odical literature may well be available in English translation. A complete list of the cover-to.
cover English translations appears at the back of, this issue.
* According to the experimental conditions, polyethylene must not be placed above the counter at the thicknesses
mentioned.
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SPECTRA OF FAST PILE NEUTRONS IN PASSAGE THROUGH POLYETHYLENE
V. N. Avaev, G. A. Vasil'ev, A. P. Veselkin, Yu. A. Egorov,
Yu. V. Orlov, and Yu. V. Pankrat'ev
Translated from Atomnaya Energiya, Vol. 15, No. 1.
pp. 20-22, July, 1963
Original article submitted August 25, 1962
A single-transducer fast-neutron spectrometer was used to measure the spectra of fast pile neutrons
after passing through polyethylene layers of different thicknesses. The results of measurements at
En> 3 MeV show excellent agreement with data computed by the method of moments. At En< 3
MeV, the discrepancies are accounted for by the difference in the geometry and in the original
spectra. Problems involving the correct procedures to be followed in setting up experiments of this
type are discussed.
The measurement of the deformation of spectra of fast pile neutrons after their passage through shielding ma-
terial is a complicated experimental task, and only a scant number of papers have been published throwing any light
on the results of experiments in this line [1]. The problem is that the fast flux is accompanied by high-level gamma
flux, and until recently no highly efficient fast neutron spectrometer capable of reliable operation in the presence
of considerable gamma background was known. Research on the dependence of scintillator deexcitation time on
the mode of the emissions being recorded has led to such a spectrometer becoming available [2].
In the experiments, conducted by the present authors, the spectra of fast neutrons passed through polyethylene
were measured in a barrier-geometry water-cooled water-moderated research reactor. Slabs of polyethylene 680
x 680 x 10 mm3 were positioned in recesses in the reactor shielding. The polyethylene slab.thickness increased in
the direction of the spectrometer transducer in the course of the measurements. Measurements were performed with
the aid of a single-transducer fast-neutron scintillation spectrometer, and discrimination of gamma background was
carried out by means of the space charge between the last dynode and the anode of the photomultiplier tube [2].
The spectrometer transducer contained a FEU-33 photomultiplier and a stilbene crystal 30 mm in diameter and 20
mm high. The fast spectrum was determined by the amplitude distribution of pulses due to recoil protons in the
stilbene crystal. The amplitude distribution of pulses was transformed into the energy distribution of neutrons through
a procedure proposed by Broek and Anderson [3]; corrections for secondary scattering of neutrons in the crystal and
for partial leakage of recoil protons out of the cyrstal were introduced into the energy distribution so obtained.
Investigation of the spectrometer gamma-sensitivity revealed that the spectrometer failed to record gamma
emission at a dose rate lower than 20 pr/sec. A slab of lead 16 cm thick was placed in front of the polyethylene,
therefore, with the object of reducing the gamma intensity issuing from the pile, and the spectrometer transducer
was placed in paraffin shielding with boron and lead in such a way that it could "see" almost the entire surface of
the polyethylene slab. Boron-loaded polyethylene (0.5 wt. %) was employed to reduce capture gamma radia-
tion in the polyethylene and to cut down the thermal flux. In addition, a 5 cm thick layer of bismuth* was placed
directly in front of the transducer.
However, as the thickness of the polyethylene increased, the ratio of neutron flux to gamma flux declined
drastically in value, and even at a gamma recording efficiency (Co60)of 0.005% and neutron recording efficiency
(Po+Be) of 44%, the contribution of pulses due to recording of gamma emission became conspicuous even at poly-
ethylene thicknesses ranging from 30 to 90 cm. It was established in the cource of the experiments that the gamma-
ray background,discrimination level at 1.33 MeV maximum energy is insufficientto discriminate against high-en-
ergy gamma photons. Pulses due to electrons of -3 MeV and higher are clearly observed in the amplitude distribu-
tion, and their effect was evaluated by means of a paraffin filter 20 cm thick places in front of the spectrometer
transducer.
* It has been shown experimentally that a slab of bismuth 5 cm thick will not deform the fast neutron spectrum at
En> 2.5 MeV; at En < 2.5 MeV the deformation of the spectrum is not greater than 20%.
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6
2
107
'I.
8
6
2
20 0
Neutron energy, MeV
Spectra of fast neutrons passed through polyethylene:
1) spectrum of fast pile neutrons passed through 16 cm
lead; 2, 3, 4, 5, 6) spectrum of fast pile neutrons passed
through polyethylene of 10, 20, 30, 60, 80 g/cm2 thick-
ness, respectively. Filled data points indicate data ob-
tained at Ent = 0.6 MeV; hollow data points denote data
obtained at En2= 2.1 MeV.
In order to avoid any distortions due to the gamma-
ray background, and at the same time to measure the
spectrum over the broadest possible-range of fast-neu-
tron energies, all of the experiments were carried out
at the two energy thresholds of the spectrometer:*
En1= 0.6 MeV and Ent = 2.1 MeV. At the threshold
EnZ= 2.1 MeV, the pile gamma radiation escaped de-
tection.
After the results were processed, it was found that
the spectral distribution obtained at threshold Ent was
slightly lower than that obtained at threshold EnZ,
the discrepancy amounted to 15-20% in the 3-5 MeV
energy range. The results obtained at En2 were accepted
as the actual values, i.e., when the spectrometer failed
to record gamma emission; and the Ent results were ac-
cordingly increased by 15-20%. The differential fast
spectra so obtained in the energy region to 10 MeV ap-
pear in the accompanying diagram.
Errors in the measurements consisted of statistical
errors, errors in determining the energy threshold (f0.1
MeV), errors in determining the reactor power level,t
in determining the polyethylene thickness and density,
and also of errors related to imprecise calibration of
the spectrometer. The errors indicated in the diagram
are the sum of the statistical errors and of the errors in
determining the energy threshold. Other errors were
substantially less in our estimation, and were therefore
left out of account.
The measured fast spectra (denoted by points on
the diagram) were compared with results predicted by
the method of moments [4] on the neutron spectra of a
point isotropic fission source in the polyethylene (in-
dicated by solid curves on the diagram). For purposes
of comparison, experimental results were normalized
with the predicted data at a polyethylene slab thick-
ness of 20 g/cm2 and neutron energy of 6 MeV.
.Clearly, from the diagram, the spectrum of fast
neutrons emitted by a reactor and passed through a slab
of lead is slightly different from the fission neutron spec-
trum at En < 3 MeV; at En> 3 MeV, the measured spec-
trum agrees with the fission spectrum within the limits
of experimental error.., The difference between the meas-
ured spectrum and the fission spectrum at En < 3 MeV
may be ascribed to the following factors: 1) distortion
of the fission spectrum in the reactor core in response
to neutron scattering; 2) the difference between the
geometry of the experiment and the geometry adopted
in the calculations; and 3) the presence of a lead shield.
* The spectrometer energy thresholds were determined from the results of measurements of (d, d)-neutron spectra.
t The reactor power level varied by a factor of 104 during the measurements, depending on the thickness of the poly-
ethylene slab.
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However, to judge by the energy dependence of the removal cross section in the case of lead [5], the presence of
this shield should not lead to such a distortion of the spectrum.
The measured spectra show excellent agreement, at all polyethylene thicknesses in question, with predicted
results at En> 3 MeV. At En< 3 MeV, a certain discrepancy is observed between the measured and the theoretically
predicted spectra, on account of the difference in the initial spectra. The tendency of the spectrum to change in
that range of energies as the thickness of the polyethylene increases is the same as that found in the predicted spec-
tra. At neutron energy 3-4 MeV and at polyethylene slab thicknesses greater than 20 g/cm2, a steeper decline is
seen in the measured spectra than in the theoretically predicted spectra. This is apparently related to the inaccurate
choice of, or averaging of, the cross sections in the calculations. The same steep decline was detected in measure-
ments of neutron spectra in water [1].
The authors take this opportunity to express their gratitude to the.reactor operations staff and to the laboratory
technicians for their kind assistance in the performance of the experiments herein described.
1. USAEC Manual. Research Reactors(1956).
2. R.. Owen, IRE Trans. Nucl. Science, NS-5, 198 (1958).
3. H. Broek and G. Anderson, Rev. Sci. Instr., 31, No. 10 (1960).
4. H. Goldstein, Fundamental aspects of reactor shielding, Addison Wesley, Cambridge, Mass. (1959).
5. B. I. Sinitsyn and S. G. Tsypin, JAE, 12, 306 (1962).
All abbreviations of periodicals in the above bibliography are letter-by-letter transliter-
ations of the abbreviations as given in the original Russian journal. Some or all of this peri-
odical literature may well be available in English translation. A complete list of the cover-to-
cover English translations appears at the back of this issue.
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THE SEPARATION OF Zr95, Nb95, and Ru106 FROM A MIXTURE
OF FISSION PRODUCTS BY EXTRACTION WITH TRIBUTYL PHOSPHATE
N. E. Brezhneva, V. I. Levin, G. V. Korpusov,
E. K. Bogacheva, and N..M. Man'ko
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 23-30, July, 1963
Original article submitted July 6, 1962
We have studied methods for preparing radiochemically pure isotopes of -Zr95, Nb95, and Ru116 by a
previously described [1] general scheme for the separation of fragmentary radioactive elements.
We mainly consider regularities which were established in a study of the extraction of zir-
conium, niobium, and ruthenium by tributyl phosphate (TBP).
Ruthenium is extracted by TBP after preliminary concentration on the sulfides of metals.
Niobium and zirconium are separated by successive reextraction of niobium by hydrogen
peroxide and zirconium by oxalic acid.
Methods of Experiments
The extraction of zirconium, niobium, and ruthenium was studied under static conditions by shaking solu-
tions in separating funnels; for the dynamic conditions we used a glass extraction semicountercurrent apparatus con-
sisting of 20 sections. We used pure preparations of radioactive isotopes of Zr95, Nb95, Ru106Y91 Eu152, and Eu154 to
lable the solutions.
TABLE 1. Kdistr of Zirconium and Niobium Between TBP and Aqueous Solutions of Nitric Acid at 20?C
Zirconium
Equilibrium concentration of
HNO;1, M . . . . . . . . . . . . . . . 1,3 3,7 4,6 8,1 9, 7 11,2 13,5
Kdistr . . . . . . . . . . . . ... . . 7,5 18 25 66 109 217 270
Niobium
Equilibrium concentration of
IINO.;, M . . . . . . . . . . . . . . . 2,6 4,6 5,4 6,4 7,9 8,5 9,3 9,5 10,5 12,2 15,3
Kdistr . . . . . . . . . . . . . . . . 0,9 1,2 1,5 2,15 3,6 4,3 4,5 4,8 :i,9 11,2 24
Zirconium
;Equilibrium concentration of
HNO3, M . . . . . . . . . . . . . . . 0,9 2,0 5,1 6,2 8,0 9,1 10,2 11,1 12,2
Kdistr . . . . . . . . . . . . . . . . 0,03 0,09 1,1 3,4 5,0 9,3 17,3 22,8 85,3
!Niobium
,Equilibrium concentration of
1lN03, Al . . . . . . . . . . . . . . . 1,4 2,4 3,2 .4,3 5,6 6,9 7,2 10,3
Kdistr . . . . . . . . . . . . . . . . 0,009 0.02 0,04 0,09 0,13 0,23 0.42 0,93
In the dynamic experiments the solution under investigation, containing a mixture of isotopes in nitric acid
of a certain concentration, was placed in the first section of the extractor described in [1]. We poured wash solu-
tions of the appropriate composition into the remaining sections. TBP which had first been brought to equilibrium
with the aqueous phase was passed through the extractor. Samples of solvent leaving the apparatus and also the con-
tents of the extraction cells were subjected to radiometric analysis at the end of the experiment.
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A I I
2 3 45678510
Concentration of TBP, %
Fig. 1. Dependence of the coefficient of dis-
tribution of niobium between nitric acid and
a mixture of TBP and benzene on the TBP
concentration (tan a = BC 154 AC 96 = 1.64).
E
0
o
N
0
N 150
Extraction of Zr95 and Nb95
We studied the dependence of Kdistr of zirconium and nio-
bium in extraction by undiluted TBP and 40% solution of TBP
in kerosene (Table 1) on a number of factors. On extraction by
diluted TBP, Kdistr of niobium increases in proportion to the sec-
ond power (approximately) of the TBP concentration in the or-
ganic phase (Fig. 1). This shows that the extracted complex in-
cludes two TBP molecules. Bearing in mind the increase in Kdistr
with increase in acidity, we can assume that HNO3 molecules
also take part in the formation of the extracted complex.
A feature of the behavior of zirconium and niobium is the
apparent irreversibility of the distribution. For example, Kdistr
during reextraction is much higher than during extraction.
TABLE 2. Dependence of Kdistr of Nio-
bium on the Holding Time of the Solution
Holding
time, h
0
24
48
72
96
216
264
Kdistr
0,49
0,69
0,34
0,25
0,15
0,05
0,71
0,89
1,05
0,91
0,88
0,59
0,32
The existence of several chemical forms of zirconium and
niobium in solutions is shown by data obtained during extraction
and reextraction in successive portions from one solution (Fig. 2).
The values of Kdistr of niobium in three successive extractions
from the same portion of solution are 8.2, 1.4, 0.9, respectively.
On the other hand, Kdistr of niobium depends on the time the
solution is kept (Table 2) after its preparation (by dilution of a
solution of niobium in concentrated HNO3).
These data show that both phases contain several chemical
forms of zirconium and niobium, the equilibrium between which
1001 1 1 1 1 is established with a relatively low rate. The difficulty in the
1 2 34
reextraction of zirconium and niobium is readily overcome by
using complex formers: hydrogen peroxide for niobium and oxalic
Fig. 2. Distribution coefficient of zirconium acid for zirconium. Experimental data on reextraction with com-
during successive reextractions from TBP. plex formers are given in Tables 3 and 4. It can be seen that an
increase in HNO3 concentration above 13 N for niobium and
above 5 N for zirconium prevents reextraction. Hydrogen peroxide does not affect the distribution of zirconium.
Extraction of Zirconium and Niobium Under Dynamic Conditions
In a glass extractor we experimented on the separation of an artificially prepared mixture of zirconium with
niobium. The first section contained a mixture of Zr95 and Nb95 in 10 N HNO3 in the second and third sections there
was 10 N HNO3, containing 2% H2O2. Through the system we passed TBP in equilibrium with 10 N HNO3. When the
experiment was completed we measured the activity of the contents of the sections and obtained absorption curves
for the. radiation of aqueous phases from sections with H202 and the last portion of solvent leaving the apparatus. The
absorption curves would seem to show that the reextracted niobium.does not contain noticeable impurities of zir-
conium and the latter is not contaminated with niobium.
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TABLE 3. Reextraction of Zirconium by HNO3 Containing Complex Formers (1% H202 or 0.1% H2C204)
Equilibrium concentra-
tion of HNOg in aque-
ous phase, lVl
5,3
8,0
1,0
1,45
2,5
5,3
5,8
6,7
7,7
Complex
former
H202
H202
H2C2O4
H2C204
H2C204
H2C204
H2C2O4
H2C204
H2C204
Kdistrduring reextractio
380
400
10-3
0,005
0,004
0,52
1,7
4,7
21,4
TABLE 4. Reextraction of Niobium by HNO3 Containing Complex Former (1% H202)
Equilibrium concentra-
tion of HNO3 in aque-
ous p
phase, M
-
Kdistr during reextrac
tion
Degree
of reextrac-
tion,
%
'0 2
8
6
4
V 6
2,6
6,8
7,3
9,3
10,5
12,0
13,0
14,6
16,5
0,11
0,1
0,1
0,1
0,13
0,20
0,35
7,0
11,0
90
91
91
91
89
83
74
13
8,3
100 200 300 400 500 600 700 800 2
91, mg/cm
Fig. 3. Curves for absorption of radiation of Zr95
and Nb95 preparations obtained in an experiment
with an extractor: a) pure Zr95; 2) pure Nb95; ?)
Zr95 preparation; 0) Nb95 preparation.
The results formed the basis for the dynamic extrac-
tion separation of zirconium and niobium from a nitric acid
solution of an iron hydroxide precipitate obtained during the
treatment of mixtures of fission products according to the
scheme of [1].
For this purpose we used an extractor with 19 sections.
The first section contained the initial solution with 9.8 N
HNO3, the next four contained HNO3 to remove from the TBP
radioactive elements which were extracted less efficiently
than zirconium and niobium; the next four sections contained
HNO3 with 2% H202 to reextract the niobium. For the re-
extraction of zirconium, the sections with 1 N HNO3, in-
tended for the washing out of impurities, were followed by
sections containing 2 N HNO3 and 1 N oxalic acid. We passed
TBP in equilibrium with 9.7 N HNO3 through the extractor.
In Fig. 3 curves for the absorption of radiation of the reex-
tracts, containing zirconium and niobium, are compared with
curves for the absorption of radiation of the pure preparations.
An analysis of the wash sections showed that impurities
of radioactive cerium and yttrium contained in the initial
nitric acid solution are concentrated in them.
Extraction of Ru106
The main regularities of the distribution of ruthenium
during extraction were studied with preparations of pure radioactive ruthenium. To prepare extracted complex of
nitrosyl ruthenium we must have oxide of nitrogen or compounds which readily liberate them, for example nitrous
acid. Special experiments, the results of which are given in Fig. 4, showed that in the presence of N02 ions during
extraction by TBP from nitric acid solutions Kdistr of ruthenium at first increases and then falls sharply. With in-
crease in the concentration of NO" ions the value of Kdistr of ruthenium continuously increases (Fig. 5). A study
of the distribution of ruthenium as a function of the acidity showed that Kdistr of ruthenium passes through a sharp
maximum (Fig. 6). During repeated extraction from the same solution over certain intervals of time Kdistr of ru-
thenium continuously decreases (Table 5).
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Kdistr
Kdistr n 15
Fig. 4. Dependence of Kdistr of
ruthenium between TBP and HNO3
on the nitrite ion concentration in
the aqueous phase.
1 2 3 It 5 [NoNOJV
10 [NNO
Fig. 6. Depdendence of Kdistr of ru-
thenum between TBP and nitric acid
on the concentration of the latter.
Fig. 5., Dependence of Kdistr of ru-
thenium between TBP and nitric acid
solution on the nitrate ion concentra-
tion (at constant ionic strength).
;S 0 0,1 0,2 0,3
log[NNQ?]
Fig. 7. Extraction of ruthenium by TBP
from solutions of varying acidity: 1)
primary extraction; 2) secondary extraction.
As can be seen from Table 5 and Fig.7, with increase in the acidity of the solution the differences in Kdistr
during primary and repeated extractions decrease and eventually disappear completely.
In successive reextractions from the organic phase after short intervals of time the values of Kdistr gradually
increase even when an active reextracting medium is used, such as a 2 N solution of ammonium carbonate. In this
case Kdistr for two successive reextractions is 0.175 and 0.270.
As can be seen from Fig. 8, increasing the concentration of HNO3 during reextraction leads to a reduction in
the values of Kdistr? The values of Kdistr for ruthenium during extraction increase with increase in the content in
TBP of its hydrolysis products, forming intensively, especially during heating with acid.
Concentrating Ru106 on Sulfide Precipitates. The conditions for the occlusion of radioactive ruthenium by pre-
cipitates of nickel, copper, and cadmium sulfides were studied as a function of the amount of carrier, the excess
concentration of ions of precipitating agent, the temperature and concentration of the added reducing agent. As
can be seen from Table 6, the best results are obtained using precipitates of nickel and copper sulfides. Lead sul-
fide is less convenient due to difficulty in dissolving this precipitate. Adding up to 1 g/liter of hydrazine to the
solution does not affect the extraction of ruthenium.
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Kdistr
5
Separation of Radioactive Ruthenium From a
Solution of a Mixture of Fission Products. Using the
described method, we separated radioactive Ru106 from
the decanted oxalate solution obtained in the treat-
ment of a mixture of long-lived radioactive isotopes.
The washed precipitate of nickel sulfide ob-
tained from the decanted oxalate solution was dis-
solved in HNO3; the acidity was reduced to 0.2 N by
the addition of caustic alkali; after adding sodium ni-
trite to a concentration of 0.2 N, we extracted the
solution with TBP in equilibrium with 0.2 N HNO3.
The results for the extraction of radioactive ru-
thenium are given in Table 7; the best results were
obtained for nickel and copper sulfides.
A simultaneous study of the extraction of nickel
and copper showed that Kdistr for these elements is
0.05 and 0. 12, respectively.
The degree of extraction of radioactive ru-
thenium from a sulfide precipitate is therefore not
less than 80%
Discussion of Results
The value of Kdistr of zirconium between TBP
and HNO3 increases continuously with increase in con-
centration of the latter, without passing through a
maximum, which is the case in the extraction of many
other elements. The same regularity was observed by
other investigators studying the extraction of zircon-
ium [2-4]. It is of course possible that the maximum
nevertheless exists, but that it is beyond the limits of
the investigated region of HNO3 concentrations. Its
appearance on the curve for the dependence of Kdistr
on the acid concentration is usually connected with a
reduction in the concentration of free solvent due to
its combining with the extracted acid, or with the
formation in the aqueous phase of unextractable com-
plexes of the distributing element with the anion of
the acid.
HNO3 concentration
Fig. 8. Values of Kdistr for ruthenium between TBP and
HNO3 during reextraction from the organic phase (the
HNO3 concentration in the aqueous phase is plotted along
the abscissa axis).
TABLE 5. Change in Kdistr of Ruthenium During Re-
peated Successive Extraction From the Same Solution
Number of First series of
extraction experiments
Second series ofj
experiments
1 0,641 0,58
0,27 0,27
3 0,23 0,20
4 0,20 (l, (i(i*
0,13
? Solution treated with 24 N HNO3.
TABLE 6. Dependence of the Occlusion of Radioactive
Ruthenium by Sulfide Precipitates on the Nature of the
Carrier (Concentration of Carrier 3.4 mM)
Occlusion of ra-
Concentration of
I dioactive ruthen-
sodium sulfide, M ium by precipi-
tate, 16
Ni
0,1
99,2
Cu
0,1
98,2
Pb
0,1
98,2
Cd
0,1
91,0
N i
0,02
20
Cu
0,02
24
Pb
0,02
7,5
(Id
0,02
9,0
B i
0,02
9,0
Sb
0,02
1.5
We were unable to obtain sufficiently precise
data on the composition of the extracted complex of
zirconium. It can be assumed that these complexes
are the neutral molecule of Me(NO3)4 or the complex
acid H2Me(NO3)5.
Some investigators [2, 4] who have studied the
extraction of zirconium believe that this element trans-
fers to the organic phase in the form Zr(NO3)4 ? x TBP. However, according to the data of [5], Kdistr of zirconium
for a constant concentration of NOg ions increases approximately proportional to the second power of the H+ ion
concentration. The authors of[ 5] attribute this phenomenon to the suppression of hydrolysis of zirconium or the
formation of the complex H2Me(NO3)~ ? x TBP. The first explanation is unlikely since at acid concentrations of 3-5
N, at which the investigation was conducted, microquantities of zirconium are hardly hydrolyzed at all [6, 7]. A. M.
Rozen and co-workers explain the. regularities of extraction of zirconium at high acidities by the formation of com-
plexes of the type Zr(NO3)4 ? mHNO3 [8].
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TABLE 7. Extraction of Radioactive Ruthenium by TBP There is disagreement in the literature with re-
From a Solution of Sulfide Precipitates of Various Metals gard to the number of TBP molecules in the extracted
1Occlusion of zirconium complex. According to [2] the number of
to6 Extraction of TBP molecules in the solvate is equal to two. In an-
Carrier Ru by pre Kdistr 106 ?/o other [4] a formula of Zr(NO
cipitate, % Rti paper 3)4 ? (TBP)3 is given
_._; for the composition of the complex. Data are also
Ni
98,3 4,6
82
.:u
98,2 40
80
Pb
)8,0 i 3,1
76
cd
11,0 0,45
31
favoring the formula Zr NO TBP ? xHNO3 In
g ( 3)4' s [9].
our opinion the most convincing are the data of [8];
for three nitric acid concentrations (0.5, 4, and 9 M),
curves were obtained with the tangent of the slope close
to two, indicating the following composition of the
extracted complex:
Zr(N03)4. nITNO3.2TBP.
The absence of a maximum on the curve of Kdistr versus acid concentration for a complex of this composition
points to the relative instability of the higher nitrate complexes of zirconium (for example, compared with similar
complexes of cerium or plutonium).
A characteristic feature of the extraction of zirconium is its apparent irreversibility. For the same composi-
tion of the phases Kdistr of zirconium is much greater if the zirconium was initially in the organic phase (reextrac-
tion) than in the case where it was initially added to the aqueous phase (extraction).
These phenomena could be explained by hydrolysis on the basis of the fact that the zirconium forms a stable
hydrolytic complex in weakly acid solutions [10-12]. The hydrolysis if accompanied by polymerization and the re-
verse process of depolymerization of zirconium, like plutonium [14], proceeds slowly and with difficulty. Hydrolysis
undoubtedly affects the extraction of zirconium and is very important for low acidities; however, the "irreversi -
bility" is also observed at high HNO3 concentrations, when the hydrolysis can be neglected. There is more likely
to be a strong chemical reaction between the TBP and the extracted zirconium, leading to the formation of stable
complexes of zirconium with the decomposition product of TBP-dibutylphosphoric acid. This chemical reaction
proceeds at a measurable rate and Kdistr during reextraction therefore has unstable values, increasing at each of
the subsequent stages of reextraction. The reaction of zirconium with the decomposition products of TBP is also
shown by the increase in Kdistr with time when an insufficiently purified solvent is used [2].
Niobium is hydrolyzed to a still greater extent than zirconium [15-17]. Equilibrium between various products
of hydrolysis and the ionic forms of niobium is sometimes established extremely slowly. Hydrolysis causes a slow
reduction in Kdistr, lasting many hours and days. In solutions of niobium the unextracted hydrolytic polymers and
also colloidal (or pseudocolloidal) forms exist at comparatively high acid concentrations [18]. This is due to the
change in Kdistr during repeated extractions from the same aqueous solution: after each extraction the fraction of
hydrolytic complexes in the solution increases and Kdistr decreases. With increase in the HNO3 concentration the
value of Kdistr for niobium does not pass through a maximum.
Since the extracted form of ruthenium contains, in addition to the nitrate ion, the nitroso group NO [19, 20],
for the formation of a nitrosyl-ruthenium ion RuNO3+ we must evidently have lower oxides of nitrogen or compounds
which readily liberate them, for example, nitrous acid. In fact, in the presence of nitrites Kdistr for ruthenium in-
creases sharply. However, nitrite ions also have a negative effect on the extraction: with increase in their concen-
tration there is an increase in the fraction of unextracted nitrite complexes of the type RuNO(NO2)3 [20-24]. Kdistr
of ruthenium therefore increases at first with increase in the nitrite ion concentration, passes through a maximum
and then again decreases.
Among the nitrate complexes formed by nitrosyl ruthenium, the greatest extractability is shown by the satur-
ated neutral complex RuNO(NO3)3 [19, 25] the fraction of which naturally increases with the HNO3 concentration
[19-20] and the N03 ions in general. This explains the increase in extraction of ruthenium with increase in the
NaNO3 concentration.
The extraction of ruthenium is very sensitive to the acidity of the solution. During extraction from HNO3 solu-
tions of varying concentration Kdistr for ruthenium passes through a fairly sharp maximum (see Fig. 6).
From data on the study of extraction it also follows that at low acidity, corresponding to the greatest extrac-
tion of ruthenium, the latter is in solution in several chemical forms, equilibrium between which is established
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slowly. Similar conclusions are drawn by other investigators [19, 25]. During repeated extraction from the same
solution Kdistr for ruthenium continually decreases after short intervals of time (see Table 5) since after each ex-
traction there is a reduction in the content'of the most readily extracted forms. The readily extracted form is
RuNO(NO3)3, and the difficulty extracted forms are the lower nitrate complexes [19, 20] and different stages of
hydrolysis of nitrosyl ruthenium and its nitrate complexes [19, 26].
Accordingly, with increase in the acid concentration differences in Kdistr during primary and secondary ex-
tractions decrease and finally disappear altogether (see Fig. 7).
In the organic phase ruthenium is also found in various forms with differing stabilities in combination with
TBP. During successive reextractions from the organic phase, after short intervals of time the values of Kdistr there-
fore gradually increase, even when an ammonium carbonate solution is used.
The extracted complex of ruthenium RuNO(NO3)3 in the organic phase gradually changes to other compounds
which are more firmly combined with the solvent.'. As in the extraction of zirconium and niobium, we can assume
slow extensive reaction of ruthenium with TBP or its decompostion products. This is confirmed by the fact that
Kdistr of ruthenium during extraction increases with increase in the content of TBP hydrolysis products in the or-
ganic phase.
The results given here for the separation of radioactive zirconium, niobium, and ruthenium from solutions re-
maining after the separation of a calcium oxalate precipitate indicate that the complex method [1] which we have
developed can be used to obtain radiochemically pure preparations of these fission products.
The concentration of zirconium and niobium on a hydroxide precipitate is not an unusual operation. Less
usual is the concentrating of ruthenium on sulfides. This method enables ruthenium to be more completely sep-
arated from solution. The absorption of radioactive ruthenium by sulfides of metals was also described in [27, 28].
LITERATURE CITED
1. N. E. Brezhneva, V. I. Levin, G. V. Korpusov, et al., In: Transactions of the Second International Conference
on the Peaceful Uses of Atomic Energy. Report of Soviet Scientists. Vol. 4, Moscow, Atomizdat, p. 57 (1959).
2. K. Alcock, et al., J. Inorg. and Nucl. Chem., 4, 100 (1957)."
3. D. Peppard, et al., J. Inorg. and Nucl. Chem,, 3, 215 (1956).
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5.
6.
7.
8.
G. F. Egorov, V. V. Fornin, Yu. G. Frolov, and G. A. Yagodin, Zh. neorganich. khim., 5,
1044
(1960).
A. S. Solovkin, Zh. neorganich. khim., 2, 611 (1957).
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N. M. Adamskii, S. M. Karpacheva, I. N. Mel'nikov, and A. M. Rozen, Roadiokhimiya, 2, 400
(1960).
9. Z. N. Tsvetkova, A. S. Solovkin, N. S. Povitskii, and I. N. Davydov, Zh. neorganich. khim., 6, 489 (1961).
10. R. Connick and W. Reas, J. Amer. Chem. Soc., 73, 1171 (1951).
11. K. Kraus and J. Johnson, J. Amer. Chem. Soc., 75, 5769.(1953); 78, 3937 (1956).
12. V. I. Paramonova and A. S. Voevodskii, Zh. neorganich. khim., 1, 1905 (1956).
13. I. E. Starik, I. A. Skul'skii, and A. I. Yurtov, Ra.diokhimiya, 1,. 66 (1959).
14. A. Brunstad, Industr. and Engng. Chem., 51, 38 (1959).
15. J. Kanzelmeyer and J. Ryen, J. Amer. Chem. Soc., 78, 3020 (1956).
16. V. I. Paramonova, et al., Zh. neorganich. khim., 3, 212 (1958).
17. I. E. Starik and I. A. Skul'skii, Radiokhimiya, 1, 77 (1959)..
18. V. I. Paramonova and V. B. Kolychev, Zh. neorganich. khim., 1, 1896 (1956).
19. J. Fletcher, Progr. Nucl. Energy, Ser. III, Process Chem., 1, London, p. 105 (1956).
20. A. Wain, P. Brown, and J. Fletcher, Chem. Ind., No. 1, 18 (1957).
21. O. E. Zvyagintsev and S. M. Starostin, Zh. neorganich. khim., 2, 1281 (1957).
22. J. Fletcher, J. Inorg. and Nucl. Chem., 1, 378 (1955).
23. J. Fletcher, J. Inorg. and Nucl. Chem., 8, 287 (1958).
24. F. Martin, et al., J. Chem. Soc., 76 (1959).
25. V. D. Nikol'skii and V. S. Shmidt, Zh. neorganich. khim., 2, 2746 (1957); 3, 2967 (1958).
26. I. Jenkins and A. Wain, J. Inorg. and Nucl. Chem., 3, 28-37 (1956).
27. F. Martin and J. Miles, Progr. Nucl. Energy, Ser. III Process Chem., 1, London, p. 369 (1956).
28. F. Martin and J. Miles, AERE, C /R 2413 (1957).
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Sh. Sh. Ibragimov, I. M. Voronin, and A. S. Kruglov
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 30-37, July, 1963
Original article submitted May 31, 1962
We have studied the effect of neutron irradiation at temperatures of 200-500?C with various integral
.doses (1.5' 10E0-7. 1021 neutrons/cm2) on the properties and microstructure of some steels with differ-
ent chemical compositions and initial structures. We have shown the effect of alloying by various
elements on the sensitivity of the steel to irradiation and the temperature of annealing of radiation
defects of hardening.
In recent years a number of papers have been published [1-6] on the effect of neutron irradiation on the me-
chanical properties of low- and complex-alloy steels. Nevertheless,'he existing data are far from sufficient to ex-
plain the effect of alloying by elements and the initial structure of the steel on the change in its properties during
irradiation. There is comparatively little information on the change in mechanical properties of steels during ir-
radiation by high integral doses (above 5.1020 neutrons/cm2). To a certain extent the present work extends our ideas
in this field. -
Material and Irradiation
We studied iron and steel (2Kh2MS, 2Kh6MST, 1Kh12MS, 1Kh16MSB, 1Kh18N9T, and 1Kh18N14MSB), differ-
ing considerably from one another in their chemical composition and the phase-structural state.
Tnteoril flnv
Strength,
kg/mm 2
;temperatures,
?C
I
Neutrons with
E >tMeV
Yield point
during 0.2%I Relative
deformation, elonga-
kg/mm tion, ojo
Iron, annealed at
I 760?C
200-240
200-240
200-240
200-240
0
1,1.1020
1.5.1020
1 9.1020
2.8.1020
0
1,1.1019
1,5.1019
1,9.1019
2,8.1019
35,0
50,0
52,0
52,5
53,5
29,5
49,5
51,5
51,5
52,5
38,5
18,5
15,5
15,0
16,0
1Kh16MSB steel, annealed
?
0
0
63,0
44
0
26
0
at 900
C
200-240
1,5.1020
1,5.1019
73,0
,
58,0
,
19
1)
200-240
1,9.1020
1,9.1019
74,0
60,0
,
12
0
200-240
2,8.1020
2,8.1019
74,5
65,5
,
8
0
200-240
8.1020
8.1019
75,0
66,0
,
8
0
320-360
1,2.1021
3.6.1020
74,5
56,0
,
10
0
450-500
7.1021
2,1.1021
65,5
50,0
,
24,0
1Kh16MSB steel has a ferrite structure with stable carbides; 2Kh2MS, 1Kh6MST, and 1Kh12MS steels are ferritic
perlitic and the remainder are austenitic.
From bars of these materials we prepared small tensile specimens, with a diameter of 3 mm in the calculated
part and a total length of 25 mm; the specimens were used for the tensile tests, metallographic analysis, and the de-
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terminations of hardness. From steels of some grades specimens were prepared in the form of 2-mm diam wire
to study the electric resistance.
All the specimens were annealed before irradiation in the reactor. Furthermore, to find the effect of the in-
itial microstructure on the change in mechanical properties during irradiation specimens of steels of some grades
were subjected to varying heat treatment. The heat-treated specimens in special stainless steel containers were
loaded into the BR-5 reactor [7, 8]; they were irradiated in the active zone of the reactor and two vertical channels
intended for investigation into materials. Irradiation in the active zone was carried out over a fairly "hard" energy
spectrum of neutrons (mean neutron energy 0.38 MeV; neutrons with an energy ?1 MeV comprised 3016) at tempera-
tures of 320-500?C in the channels the irradiation was conducted in a relatively "soft" spectrum (mean neutron en-
ergy 36 keV; neutrons with an energy ?1 MeV comprised 1016) at temperatures not exceeding 255?C.
TABLE 2. Mechanical Properties of Austenitic Steels and Nickel
Irradiation
Integral flux,
neutrons/cm2
-
Tensile
Yield point
during de-
form a Lion
Relative
Material
temperature,
---
strength,
elonga-
Total
Neutrons with
r. ?1 MeV
2
kg/mm
0.216,
lion, 016
kg/mm
g
1Kh18N9T steel
-
0
0
58,5
18,0
68,5
220-255
3.4019
3.1019
68,5
42,0
52,0
220-255
11021
1.1020
68,0
41,5
51,0
450-500
1,7.1021
0,5.1021
64,0
27,0
50,0
450-500
5,2.1021.
1,6.1021
70,0
33,0
58,0
1Kh18N14MSB steel
-
0
0
57,0
22,0
58,0
220-255
3.1020
3.1019
62,0
2S,0
50,0
220-255
1.1021
1.1020
68,0
38,0
30,0
450-500
1,7.1021
0,5.1021
61,5
24,5
47,0
450 500
5,2.1021
1,6.1021
I
59,5
24,0
51,0
Nickel (mean grain
-
0
0
49,0
13,5
47,0
size 6.3 mm)
200-240
1.1.1020
1.1.1019
(53,5
47,0
'29,0
200-240
1,9.1020
1,9.1019
68,5
57,5
26,0
200-2/i0
2,8.1020
2,8.1019
70,5
61,0
24,0
Irradiated and .nonirradiated specimens were tested in tension at room temperature with a remote-controlled
UMD-5 machine. Each experimental point represents a test of not less than four specimens. The hardness was de-
termined with a diamond pyramid at a load of 10 kg on a Vickers instrument adapted for operation with y-active
specimens. The microstructure of nonirradiated specimens was studied with the MIM-8 microscope; that of irra-
diated specimens was studied with the remote-controlled MIM-14 metallographic microscope.
Results of Experiments and Their Discussion
Iron and 1Kh16MSB Steel. The metallographic investigation of nonirradiated and irradiated specimens showed
that there were no noticeable changes in the microstructure of iron and steel. The ferrite grain size in both materials
is. about the same (mean diameter.-O.04 mm). The mechanical properties of the iron and steel are given inTable 1.
The data show that neutron irradiation at temperatures of 200-240 and 320-360?C considerably increases the strength and
yield point, and reduces the relative elongation of iron and 1 Kh16MSB steel. The absolute value of the change in prop-
erties depends on the temperature and integral irradiation dose. During irradiation at temperatures of 200-240?C
and below [5, 9] an intensive change in the mechanical properties of iron is observed for doses below 1.1 ? 1020 and
of steel at doses up to, 2.8 ? 1020 neutrons/cm2 (except for the tensile strength-less sensitive to radiation defects of
the characteristics). Further changes in the properties are slight; consequently, at doses of about 1.102D neutrons/cm2
for iron and 3.1020 neutrons/cm2 for 1Kh16MSB steel there is almost saturation. We notice that the maximum in-
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crease in the yield point for both materials for corresponding saturation doses has the same vaIues(22.0-23.0 kg/mm 2).
Such a change in the mechanical properties for iron and steel during neutron irradiation is connected with the forma-
tion of radiation defects of hardening in the material. In the investigated steel these defects are completely an-
nealed at temperatures below 500?C [9]. The irradiation of 1Kh16MSB steel at 450-500?C, despite the high integral
dose (7. 1021 neutrons/cm2) did not lead to a noticeable change in the mechanical properties.
TABLE 3. Mechanical Properties of 2Kh2MS Steel
Integral
flux
Irradiation neutrons
H
/cm2
Tensile
Yield
Relative
Ha
d
eat
tempera-
T
l
-
Neutrons
strength,
point,
elongation,
r
ness,
2
k
/
ota
treatment
Iture, ?C
with
2
kg/mm
2
kg/mm I
%
g
mm
E 2:1 MeV
Annealing at 1100?C -
n
0 .
95,0
71,0
16,5
-
275
and stepwise 200--240
8.10'-0
8 1019
96,0
86,0
18,0
311
cooling :320-360
1,2.1021
3,6.1020
94,5
-
5,2
297
450-500
7.1021
2,1.1021
76,0
67,0
1,0
287
The same, soaking at
0
.91,0
65,0
18,5
270
400?C for 16 days
Quenching from 1050?
-
0
0
121,0
102,0
11,0
370
in oil and tempering
200-240
8.1020
8.1019
126,5
114,5
8,5
402
at 650?C for 3 h
320-360
1,2.1021
3,6.1020
135,0
124,0
3,5
446
450-500
7.1021
2,1.1021
120,0
103,0
6,5
392
TABLE 4. Mechanical Properties of 2Kh6MST Steel
Annealing at 900?C
Irradiation
tempera-
!ture, ?C
Integral flux,
neutrons/cm2
Neutrons
with
E?1MeV
0
0
200-240
8.1020
8.1019
320-360
1,2.1021
3,6.1020
450-500
7.1021
2,1-1021
The same, soaking at
400?C for 16 days
Tensile
strength,
kg/mm2
80,0
82,0
86,5
72,5
I
Yield Relative
point, elongation,
kg /mm2 10/o
52,0
58,0
60,5
46,0
38,5
26,5
21,0
22,5
23,0
25,0
Hardness,
kg/mm2
202
254
249
Quenching from 1000?C
0
0
96,5
78,5
19,5
284
in oil and tempering
?
200-240
8.1020
8.101s
98,5
86,0
19
0
325
at 650
C for 3 h
320-360
1,2.1021
3,6.1020
101,0
,
15,5
:122
450-500
7.1021
2,1.1021
91,5.
76,0
18,0
290
The same, soaking at
71,5
20,0
282
400?C. for 16 days
Austenitic Steels and Nickel. Before being loaded into the reactor austenitic steel specimens were quenched
in water from 1100?C, and nickel specimens were annealed at 650?C for one hour. A microstructural investigation
of nonirradiated specimens showed that the austenitic grain size of the investigated steels was approximately the same
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(mean grain diameter -0.1 mm). After irradiation no changes were observed in the microstructure of the steels, only
the etchability of the grain changed. It is a characteristic fact that after irradiation twins in the austenitic grains
are either not revealed at all or are revealed as traces of boundaries of twin formation which have lost their initial
linearity.
TABLE 5. Mechanical Properties of 1Kh12MS Steel
I
di
i
Integral flux
rra
at
on
Heat
neutrons/cm
Tensile
Yield
Relative
Hardness
treatment
tempera-
?
eutrons
strength,
2
point,
elongation,
,
kg/mm2
ture,
C
Total
ith
kg/mm
2
kg/mm
%
?1MeV
nnealing at NOT
-
0
0
64,5
44,5
29,5
195
200-240
2,8.1020
2,8.1019
72,5
60,0
26,0
--
200-240
8.1020
8.1019
70,5
59,0
27,0
248
320-360
1,2.1021
.3,6.1020
74,5
62,0
25,0
243
450-500
7.1021
2,1.1021
80,0
62,5
16,0
254
he same, soaking at
-
0
0
66,5
43,5
28,5
-
400?C for 16 days
aenching from 1000?C
i -
0
0
88,5
.68,0
21,5
260
in oil and tempering !
200-240
8.1020
8.1019
93,0
82,5
19,0
312
at 650?C for 3 h
320-360
1,2.1021
3,6.1020
95,5
81,0
20,0
309
450-500
7.1021
2,1.1021
-
81,0
16,0
-
he same, soaking at
-
0
0
88,5
67,0
21,0
-
400?C for 16 days
The mechanical properties of austenitic steel and.nickel before and after irradiation by various doses at tem-
peratures of 200- 500?C are given in Table 2. The data show that changes in the properties of, investigated steels after
neutron irradiation are determined by the integral dose and the irradiation temperature and, consequently, by the
number of formed radiation defects in the material.
A certain regularity is observed in the effect of alloying elements on the sensitivity of steel to neutron irra-
diation. Complicating the steel composition by alloying with various elements, as in the case of alloying of iron, dis-
places the integral saturation flux toward a high irradiation dose. The strongest effect is therefore shown by elements
such as silicon and molybdenum. Thus, due to irradiation at temperatures of 220-255?C with an integral dose of
3' 1020 neutrons/cm2 the tensile strength and the yield point 1Kh18N9T steel increase to 10 and 24 kg/mm2, and
1Kh18N14MSB steel which, in addition to chromium and nickel, contains -117o silicon and ^-2176 molybdenum, only
increase by 5 and 6 kg/mm 2, respectively. At a dose of about 3 ? 1020 neutrons/cm2 there is almost saturation in the
change in the mechanical properties of 1Kh18N9T steel and nickel." . For 1Kh18N14MSB steel at doses of 3. 1020
1 ? 1021 neutrons/cm2 there is an intensive change in the properties and saturation evidently does not occur.
It is a well-known fact [4] that in austenitic steels irradiated at temperatures below 350?C radiation defects of
hardening are annealed in the temperature range 430-650?C. During irradiation of 1Kh18N9T and 1Kh18N14MSB
steels at 450-500?C some of the radiation defects are therefore annealed and the mechanical properties change some-
what less than in the case of irradiation at temperatures below 350?C (in both cases the integral flux exceeds the satu-
ration dose).
* When iron is alloyed with chromium and nickel the integral saturation flux is displaced toward a high dose and be-
comes the same as for nickel; this is apparently connected with the change in the crystal structure of the material
as a result of alloying. Data on the change in mechanical properties of iron and nickel as a function of the irradia-
tion dose show (see Tables 1 and 2) that, other conditions being equal, the integral saturation flux depends on the
crystal structure of the material.
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2Kh2MS, 2Kh6MST, and1Kh12MS Steels. In contrast to 1Kh16MSB steel and austenitic steels these steels are
sensitive to heat treatment; the changes in their properties during irradiation were therefore studied after two forms
of preliminary heat treatment. We also found the effect of prolonged (16 days) soaking.at 400?C on the structure
and properties of these steels.
Fig. 1. Microstructure of annealed 2Kh2MS steel (x 800): a) before -irradiation; b) after soaking at 400?C for 16
days; c) after irradiation at 320-360?C, nvt=1.2.10 neutrons/cm2; d) after irradiation at 450-500?C, nvt = 7. 1021
neutrons/cm2.
The mechanical properties of these steels are given in Tables.3, 4, and 5; it can be seen that as aresult.of
irradiation at 200-360?C there was an increase in the strength, yield point,. and.haidness, and a reduction in the relative
elongation of the investigated steels. The absolute 'value of the change in these characteristics due to irradiation
at 200-240?C (integral dose 8.1020 neutrons/cm2) was practically independent of the initial structure and properties.
As a result of irradiation at 450-500?C the strength characteristics of 2Kh2MS and. 2Kh6MST steels decreased some-
what and annealed 2Kh2MS steel almost completely lost its plasticity. Prolonged soaking at 400?C only appreciably
affected the properties oi 2Kh2MS and 2Kh6MST steels.
A metallographic study of.nonirradiated and irradiated specimens showed that irradiation at temperatures'of
320-360?C and above in a relatively hard-energy spectrum of neutrons-considerably affected the microstructure (re-
distribution, and also change in form and dimensions of the carbide phase) of 2Kh2MS and 2Kh6MST steels (Figs. 1
and 2). For 1Kh12MS steel a certain change. in the structure. is .only observed under the electron microscope and only
for the quenched-tempered state. In 2Kh2MS and 2Kh6MST steels changes in the microstructure were also observed
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after prolonged soaking at 400?C, but the form and char-
acter of these changes differ considerably from the
changes in structure due to irradiation.
We can therefore state that a change in the me-
chanical properties of 2Kh2MS, 2Kh6MST, and 1Kh12MS
steels during irradiation at 200-240?C is due to the forma-
tion of radiation defects of hardening; at 320-360?C and
above the change is due to the formation of radiation
defects and a change in the structural state of the steel
during irradiation. These defects and changes in the
microstructure do not have much effect on the electric
resistance of the steel. For example, the electric re-
sistance of annealed 2Kh2MS steel before irradiation
was 63.0 ? - 0 ? cm, and after irradiation at 320-360?C
by an integral dose of 1.2.1021 neutrons/cm2 it was 62.5
p ? 0 - cm. The radiation defects of hardening in speci-
mens of 2Kh2MS, 2Kh6MST, and 1Kh12MS steels, ir-
radiated at 200-240?C, are annealed in the same tem-
perature range 350-575?C (Fig. 3); consequently, the
temperature of annealing of the defects, as for austenitic
steels [4], is independent of the extent of alloying. We
can therefore draw the following conclusions:
1. Irradiation :of austenitic steels at temperatures
of 200-500?C by neutrons up to an integral dose of 7.1021
neutrons/cm 2 changes the mechanical properties, due
to the formation of radiation defects of hardening.
100 200 300 41)0 500 000 700
Temperature, ?C
Fig. 3. Change in the increase in hardness
of irradiated steel specimens versus an-
nealing temperature: 0) 2KhMS; 0)
2Kh6MST; 0) 1Kh12MS.
Fig. 2. Microstructure of annealed 2Kh6MST steel
(x 800): a) before irradiation; b) after soaking at 400?C
for 16 days; c) after irradiation at 320-360?C, nvt=1.2
? 1021 neutrons/cm2.
2. A change in the mechanical characteristics
of steels with a ferrite-perlitic structure (2Kh2MS,
2Kh6MST, and 1Kh12MS) during irradiation in a rela-
tively hard energy spectrum of neutrons at temperatures
of 320-360?C and above is due to the formation of ra-
diation defects and a change in the microstructure of
steel during irradiation.
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3. Complicating the composition of the material by alloying with various elements leads to a displacement
of the saturation dose toward high integral fluxes and has no noticeable effect on the annealing temperature of ra-
diation defects of hardening.
1. L. Trudo, In: Transactions of the Second International Conference on the Peaceful Uses of Atomic Energy.
Selected reports of non-Soviet scientists. Vol. 6, Moscow, Atornizdat, p. 427 (1959).
2. N. F. Pravdyuk, et al., In: Transactions of the Second International Conference on the Peaceful Uses of
Atomic Energy. Reports of Soviet scientists, Vol. 3, Moscow, Atomizdat, p. 610 (1959).
3. J. Wilson, See [1], p. 391.
4. Sh. Sh. Ibragimov, V. S. Lyashenko, and A. I. Zav, yalov, Atomnaya energiya, 8, 413 (1960).
5. D. Harries, Nucl. Power, 5, 97, 142 (1960).
6. I. M. Voronin, et al., Atomnaya energiya, 8, 514 (1960).
7. A. I. Leipunskii, et al., See [2], Vol. 2, p. 215.
8. A. I. Leipunskii, et al., Atomnaya 6nergiya, 11, 498 (1961).
9. Sh. Sh. Ibragimov and V. S. Lyashenko, Fizika metallov i metallovedenie, 10, 84 (1960).
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THE CORROSIVE EFFECT OF FUEL ELEMENT SOLVENTS
ON STRUCTURAL MATERIALS
M. M. Kurtenov and E. N. Mirolyubov
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 37-48, July, 1963
Original article submitted April 16, 1962
We examined the corrosion resistance of structural materials in boiling solutions of nitric, sulfuric,
and hydrofluoric acid, and also nitric acid with additions of fluorides with application to the tech-
nological process of dissolution of fuel'elements. The obtained data on the nature of the corrosive
action of fuel element solvents on structural materials can be used to decide on materials and
methods for protecting reactor dissolvers against corrosion.
The numerous technological schemes for the treatment of fuel elements involve very corrosive solutions.
Boiling solutions of nitric acid, nitric acid with small additions of fluorides, and also solutions of hydrofluoric
and sulfuric acids, are used as solvents for the cans and cores of various types of fuel elements [1].
A knowledge of the nature of the corrosive effect of various fuel element solvents is a very important factor
for a correct choice of structural materials for reactor-dissolvers. However, insufficient attention has been paid to
this problem in published papers.
On the basis of a thorough investigation of corrosion processes in structural materials we have shown the ex-
tent of corrosive activity of fuel element solvents, the possibility of changing it under the operating conditions of
the reactor solvent; we have also developed ideas on the mechanism of corrosion of structural materials in the above
solutions.
General Corrosion Characteristics of Metal Structural Materials
From the papers published in recent years [2-5] it follows that the corrosion of most metals and alloys in vari-
ous solutions is characterized by a certain general dependence of the steady rate of solution on the potential (Fig. 1).
On the diagram corresponding to this general dependence we can separate characteristic regions of potentials for
each of which the dissolving of materials has its own features.
Corrosion in the region of the active state (I) is characterized by an increase in the rate of solution with in-
crease in potential. In the region of partial passivation (II), on the other hand, there is a reduction in the rate of cor-
rosion with increase in potential. In the region of the stable passive state (III) the corrosion rate has a minimum
value and is independent of the potential; this is due to the chemical dissolution of the passive oxide film. In the
region of superpassivation (IV) a new increase is observed in the corrosion rate, caused by oxidation of the protec-
tive passive film to higher, more readily soluble oxides. In the region of superpassivation the corrosion rate increases
with the potential. -
The potentials of passivation ((Ppass), activation (Wa) and superpassiyation (tPsuper) bounding these regions,.
and also the anodic polarizability in the active state (tan 6) depend on the nature of the material, temperature, and
hydrogen ion concentration in the solution.
It therefore follows that the corrosion behavior of structural materials under operating conditions (extent of
corrosion, the character of its change with increase in potential and the mechanism of the process) should be deter-
mined by the region in which the stationary potential of the material will be located. The location of this potential
in a corrosive medium in a given region of potentials depends on the nature of the oxidation-reduction equilibria
in the solution, the concentration of the oxidizing agent and the overvoltage of its reduction on materials differing
in composition.
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s uper
0 g/m2 h
Fig. 1. Dependence of the corrosion rate K of struc-
tural materials on their potential in the regions: I)
active state; II) partial passivation; III) stable passive
state; IV) superpassivation.
12 16
CHN03 , M
Fig. 2. Corrosion rate of 18-8 steel with titanium
versus concentration of HNO3 solutions and tempera-
ture: 1) boiling point; 2) 60?C.
Solutions of Nitric Acid
Nitric acid solutions with concentrations up to15.8
M are used to dissolve various types of fuel element [1,
6]. Extensive use is made of 18-8 chrome-nickel steels
as structural materials when nitric acid solutions are used.
In HNO3 solutions with concentrations up to 16 M the cor-
rosion rate of this steel at temperatures up to 100?C does
not exceed 0.2 g/m2 ? h [7], since the stationary potential
of corrosion of the steels corresponds to the region of the
passive state. However, at the boiling point the corrosive
effect of the HNO3 solutions increases considerably and at
acid concentrations above 6-8 M the corrosion rate of the
steels increases sharply (Fig. 2). At these concentrations
the oxidation-reduction potential of the medium exceeds.
the potential of breakdown of the passive state in the re-
gion of positive values (`eredox> (.0 super) and according
to the mechanism of superpassivation corrosion becomes
thermodynamically possible. When the potential of steel
in a 14-M solution of HNO3 is displaced from the station-
ary state to the region of negative values the corrosion
rate decreases (Fig. 3); this is characteristic for corrosion
according to the superpassivation mechanism.
An analysis of numerous literature data on the cor-
rosion of 18-8 stainless steels in boiling concentrate d`solu-
tions of HNO3 (mainly 10-14 M) [7-12] and the results of
experiments carried out leads to the conclusion that cor-
rosion under these conditions proceeds with preferential
control* due to the retarding effect of the reduction of
HNO3 to nitrous acid and N204. Bearing in mind that the
reduction of HNO3 to nitrous acid and N204 is autocata-
lyzed by nitrous acid [13, 141 and, consequently, by ox-
ides of nitrogen which are present with the HNO2 in ra-
pidly establishing equilibrium, we can understand the rea-
sons for the strong increase in the corrosion rate of steels
in concentrated HNO3 solutions when the acid is saturated
with oxides of nitrogen [10], the accumulation in it of
products of the corrosion of steel (Fe3+, Cr6+, etc.) [8, 9],
which can be reduced cathodically, and then be oxidized
by HNO3 with the formation of oxides of nitrogen. The
acceleration of the corrosion of steels in these cases is
due to the retardation of the cathodic reduction of HNO3,
as in the case when the steels are in contact with metals
having a low overvoltage of HNO3 reduction (contact with
platinum in 12 M HNO3 during boiling intensifies the cor-
rosion of 1Kh18N9T steel by a factor of 50). These facts
are clear from the corrosion diagram shown in Fig. 4. Such
diagrams are used extensively in work on corrosion[15, 16].
It can be seen from the diagram that when the ca-
thodic process is facilitated due to the accumulation of
corrosion products in the solution or the presence of ox-
ides of nitrogen in the acid, and also due to contact with
* Near the stationary potential the cathodic polarizability is much higher than the anodic polarizability.
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platinum, the corrosion potential is displaced towardpositive values and the corrosion rate increases. With hinder-
ing of the cathodic process, for example when oxides of nitrogen are removed from the acid the potential is re-
duced and the corrosion rate falls.
It
1,2
K,g/mz?h
Fig. 3. Corrosion rate of 18-8
steel with titanium in a boil-
ing 14-M HNO3 solution versus
potential.
Fig. 4. Corrosion diagram for 18-8 steels in boiling
concentrated solutions of HNO3: `PsuperA is the an-
odic curve. The position of the cathodic curves in
the case: ~oC a) absence of oxides of nitrogen in the
solution; `PC b) presence of corrosion products in the
solution; `PC c) contact with platinum.
1 2 3
CMNOj ' N
Fig. 5. Corrosion rate of 18-8 steel with titan-
ium making contact with aluminum during dis-
solution in boiling HNO3 solutions in the pres-
ence of 0,0516 mercuric nitrate.
Fig. 6. Corrosion rate of monel
metal versus HF concentration
at 90?C: 1) in the solution; 2)
over the solution.
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Fig. 7. Corrosion rate of monel metal in HF
solutions versus temperatures: 1, 2) inside
solution; 3, 4) over solution; 1, 3) 1.6% HF;
2, 4) 14.4% HF.
It should be borne in mind that during contacting with fuel
elements which are being dissolved in boiling concentrated solu-
tions of HNO3 under the conditions of the reactor-dissolvers stain-
less steels should be corroded at lower rates than in the absence
of contact with the dissolivng metals. There is no doubt that this
retardation of the corrosion rate will be observed only if the po-
tential of dissolution of the fuel element in a given solution is more
negative than the potential of stainless steel, since only in this
case can there be cathodic protection of the steel. However, ca-
thodic polarization of stainless steel due to the contacting with
electronegative metals dissolving in HNO3, for example aluminum,
can also lead to a considerable increase in the corrosion rate of
the steel. Figure 5 gives data on the corrosion of 18-8 steel with
titanium in the boiling HNO3 solutions with additions of mercuric
nitrate in the case where this steel in in contact with dissolvingal-
uminum. For 1 g of aluminum there was 10 g of acid; the ratio
of the aluminum and steel surfaces was 6: 1. It follows from Fig. 5
that in 2-M acid the corrosion rate of steel reaches 17 p during
the dissolution operation, which lasts about one hour. The high
rate of corrosion is due to displacement of the potential of steel
(due to contact with aluminum dissolving at a negative potential,
equal to -0.8 V) in a region characterized by dissolution from the
active state. An effect similar to cathodic polarization-the break-
down of the passive state of stainless steels in HN03 solutions dur-
ing contact with electronegative metals was detected and studied
in detail in [17-20].
TABLE 1. Effect of Composition of the Gas-
eous Medium on the Corrosion Rate of Monel
Metal in Boiling 20% HF
Composition
Corrosion rate, g/m2 ? h
of medium
Inside
Over
solution
solution
Air
0.96
1.5.05
Oxygen
2.86
27.4
Argon
0.05
0.09
Hydrofluoric acid solutions are used to dissolve fuel elements
of zirconium alloys with a small content of uranium [1]. On the
basis of a study of the corrosion stability of various metals and al-
loys in HF solutions many investigators have chosen monel metal
as being the most stable structural material [1, 21-23]. However,
the literature contains no information on the mechanism of cor-
rosion of monel metal in HF solutions.
Experiments show that the corrosion rate of monel metal in
an HF solution is an order lower than that over the solution (Fig. 6).
With increase in the acid concentration and temperature the cor-
rosion rate in the solution and over the solution increases (Fig. 7)
but simultaneously remains constant with time. Similar regular-
ities are observed in the corrosion of copper. A metallographic analysis of monel metal specimens in contact with
acid for various intervals of time (Fig. 8) shows that on the surface of the specimens narrow cracks are initially
formed; these become wider with time and merge into one another, leading to continuous uneven corrosion of the
monel metal.
The corrosion rate of monel metal, like that of copper in HF solutions, depends strongly on the composition
of the gaseous medium over the solution (Table 1).
The gas which was passed over the solution was preheated to maintain isothermal conditions in the experi-
ments. The results given in. Table 1 and also the increased corrosion rate over the solution, where the oxygen of the
air has more easy access to the metal surface than inside the solution, indicate that the corrosion of monel metal
in HF solutions proceeds with oxygen depolarization with preferential cathodic control. The process of corrosion
over the solution, which develops in the film (more precisely under the drops of condensed water and acid vapors)
proceeds at a higher rate'than inside the solution; this is caused by the removal of cathodic control due to better
N. N. ?Bardizh performed the experimental part.
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TABLE 2. Corrosion Rate of Monel Metal and Copper aeration of the corroding surface. If the cathodic ion-
(g/m2' h) in 20% HF Inside the Solution as a Function ization of oxygen on metal situated above the solution
of the Presence or Absence of Contact with Semi- proceeds with a small overvoltage than that inside the
immersed Specimens solution, i.e., if the metal over the solution is a more
T
Monel metal
Copper -
emp.,
Without
With
Without
With
-
?C
contact
I contacj
A/B
contact
(contact
A/B
(B)
(A)
)_
(A)
20
0 24
,
0,31
1,3
-
-
-
40
0,65
1,0
1,5
0,38
0,85
1,5
90
0,82
3,43
4,2
1,5
4,5
3,0
effective cathode, then the contacting of the specimen
located inside the solution with another semiimmersed
specimen should evidently lead to an increase in the cor-
rosion rate of the first specimen; this is confirmed experi-
mentally (Table 2).
Electrochemical measurements show that with in-
crease in temperature and concentration of oxygen inthe
vapor phase the potential of monel metal and copper is
displaced to the region of more positive values. For cop-
TABLE 3. Stationary Potentials of Corrosion and Rate per, this follows from the data given in Table 3.
of Corrosion of Copper in 20% HF Solution. Duration Experiments show that the increase in the corrosion
of Experiments 2 h rate of monel metal and copper in hydrofluoric acid solu-
Temp.
, ?C
Atmosphere over
solution
20
40
Air
'P. V
2
0 23
0 2
7
K, g
/m
. h
0,17
0,3
4
Ox en
'' V
0,27
0.2
9
yg
K, g
z
/m? It
0,25
0,8
3
tions with increase in temperature of the solution, acid
concentration and oxygen content in the gaseous phase
so is accompanied by a reduction in the cathodic polariz-
ability of the electrodes.
0 29 Experimental data on the corrosive effect of HF
1,02 solutions with respect to monel metal and copper can
therefore be represented in a generalized form by means
of a real corrosion diagram, shown in Fig. 9.
0,36
4,7 The formation of cracks during the corrosion of
monel metal is evidently the result of the preferential de-
velopment of the corrosion process at the sites of local
stress concentration. The annealing of monel metals, relieving local stresses, completely prevents the formation of
cracks and the corrosion process develops more uniformly. The previously observed continuous uneven character of
corrosion of monel metal and copper in HF solutions is typical for processes of corrosion with oxygen depolarization
and with preferential cathodic control [24].
HNO3 Solutions with Additions of Fluorides*
Concentrated HNO3 solutions with small additions of fluorides are frequently used to dissolve various types of
fuel elements, for example, those containing plutonium, thorium, zirconium, and aluminum. Published papers on
the corrosion of structural materials in these solutions did not examine the nature of their high corrosion activity
[1, 25].
A study of the corrosion activity of such solutions over a wide range of HNO3 concentrations and additions of
ammonium fluoride up to 0.1 M showed that additions of HF, NaF, KF, etc., affect the corrosion rate of stainless
steels in HNO3 solutions in the same way as ammonium fluoride.
Figures 10 and 11 show the corrosion rates of 18-8 steel with titanium for various temperatures as a function
of the ammonium fluoride content in the HNO3 solutions. Small additions of fluoride causes a sharp increase in the
corrosion rate of stainless steel in HNO3 solutions. In relatively concentrated solutions (above 11 M) containing addi-
tions of ammonium fluoride up to 0.1 M, with increase in the fluoride content the corrosion rate changes, passing
through a maximum; with increase in the acid concentration and temperature this maximum in the corrosion rate is
displaced toward low fluoride contents. The corrosion rate remains constant with time. The corrosion has a con-
tinuous uniform'character.
The addition of sodium nitrate to concentrated solutions of HNO3 (>10-11,M) in the presence of fluoride re-
duces the corrosion rate of stainless steel (Fig. 12). With increase in the HNO3 concentration, with a constant fluor-
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ide content in the solution, the corrosion rate of stainless steels changes, also passing through a maximum (Fig. 13).
With increase in the temperature and fluoride content the corrosion rate maximum is displaced to the region of more
dilute HNO3 solutions.
Fig. 8. The character of the corrosion breakdown of monel metal in 5% HF at
90?C with time. Over solution: a) 52 h; b) 112 h; c) 372 h. In solution: d) 372 h.
C' b"
p iC, A/cm
Fig. 9. Corrosion diagram for monel metal in HF solutions.
Position of anodic curves for temperatures: (RA A) 20?C; (RA B)
40?C;t~ C) 80?C. Position of cathodic curves for atmospheres:
1) air: AC b) 20?C; JC b') 40?C; cC b") 80?C; 4C d) vapor
phase; 2) oxygen: 4, c) 20?C; 4C c') 40?C; ~ c") 80?C; 3)
nitrogen: 0, a) 20?C.
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0,06
CHF ,M
0,12
Fig. 10. Effect of ammonium fluoride additions on the corrosion rate of 18-8
steel with titanium in boiling solutions of HNO3: X) 2 M; ?) 4 M; V) 6 M; 0)
8 M; 0) 11 M; A) 12 M; C) 12.5 M; (D) 14 M.
0.02 0 04 006 0, 08 0,10
Cyr , M
Fig. 11. Effect of ammonium fluoride additions on the corrosion rate of 18-8
steel with titanium in HNO3 solutions at 95 and 55?C: ?) 6 M; 0) 8 M; 0)
12 M; x) 14 M.
From the results given in Figs. 10-13, it follows that the corrosion rate of stainless steel in HNO3 solutions with
fluoride additions depends on the hydrogen ion concentration. When the acid concentration is increased above 11 M
(see Fig. 10) and, consequently, there is a reduction in the content of hydrogen ions in solution [26], the position of
the corrosion rate maximum of steel is displaced toward lower concentrations of fluoride. The addition of nitrate
ions to the HNO3 solutions reduces the hydrogen ion concentration and the corrosion of steel (see Fig. 12). With in=
crease in temperature, a reduction in the hydrogen ion concentration in HNO3 solutions displaces the corrosion rate
maximum (see Fig. 13) toward lower HNO3 concentrations.
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12 14
CN03'M
1
2
3
4 6 8 10 12 /4 16 18 20 22 24
yn~n , M
Fig. 13. Corrosion rate of 18-8 steel with
titanium in HNO3 solutions with 0.05 M HF
as a function of the acid concentration and
temperature: 1) boiling point; 2) 60?C;
3) 20?C.
Fig. 12. Corrosion rate of 18-8 steel with titan-
ium in boiling HNO3 solutions with 0.05 M HF
as a function of the addition of sodium nitrate
to them: 0) 8 M HNO3; V) 10 M HNO3; ?) 12
M HNO3; 0) 14 M HNO3.
F -
1
F1
, 1
. 1
, 1
. 1
-]
. T
.
71
7
D
4 8 12 16 20 24 28 32 36 40 44 48 S2
g/ '-h
1
Fig. 14. Corrosion rate of 18-8 steel with titanium as a function of the
potential in 10 M HNO3 solution at 110?C with an addition of sodium
fluoride: 1) without addition; 2) 2.5 g/liter; 3) 6 g/liter.
An increase in the corrosion rate of steel with the addition of fluoride to HNO3 solutions is accompanied by a
reduction in the potential of the steel, this reduction being the greater the higher the corrosion rate. This increase
in the corrosion rate of stainless steels in HNO3 solutions with fluoride additions is observed over a wide range of po-
tentials corresponding to the region of active dissolution, the passive state, and superpassivation (Fig. 14).
The most intensive acceleration in the corrosion then occurs in the region of the passive state. Thus, on the
addition of 2.5 g/liter of NaF to 10 M HNO3 the corrosion rate of steel in the region of the passive state increases
by a factor of -80; in the region of active dissolution and superpassivation the factor is only ten. Since fluoride addi-
tions accelerate the corrosion of stainless steel to an approximately equal extent over a wide region of potentials
(with dissolution in the active state and according to a superpassivation mechanism), we can assume that the cor-
rosion. is caused by uncharged particles, for example HF molecules. In actual fact, HF is a weak acid and the con-
centration of its undissociated molecules will therefore change strongly, depending on the hydrogen ion concentration
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N
E
00
2 3 4
Me/F
Fig. 15. Corrosion rate of 18-8 steel with titan-
ium in boiling solution of 8 M HNO3 with addi-
tions of HF 0.05 M (1), 0.10 M (2), 0.15 M as a
function of the ratio of molar concentrations of
aluminum nitrate (1, 2, 3) and zirconium nitrate
(4) to fluorine.
E
b0
4 6
Cy2sp4 , M
Fig. 16. Effect of the concentration of boiling
H2SO4 solutions on the corrosion rate of
Kh23N27M3D3T steel.
in the system. It readily dissolves oxides of many metals, in-
cluding those of chromium, iron, and nickel, which exists on
the surface of stainless steels in HNO3 solutions. Consequently,
the autocatalytic acceleration of the corrosion of stainless
steels in HNO3 solutions with additions of fluorides is due to
the formation of HF molecules from fluorine and hydrogen ions;
these molecules dissolve the oxide films on the metal surface.
From the condition of a stationary corrosion rate it follows that
the rate of dissolution of the oxide film should be equal to its
rate of formation. On the addition of HF the increase in the
rate of dissolution of oxide films should therefore be compen-
sated by an increase in the growth of their formation. In the
absence of anodic polarization by an external current the only
source of oxidation of the steel can be the reduction of the
oxidizing agent (HNO3). The increase in the oxidation rate
should therefore be accompanied by an increase in the reduc-
tion current of HNO3 and, consequently, a displacement in the
potential of the steel toward negative values, which is ob-
served experimentally. In the passive state the dissolution of
steel only proceeds through a film; additions of HF or fluoride
therefore accelerate the corrosion process most strongly in the
region of potentials which characterize the passive state. Cor-
rosion in HNO3 solutions with HF additions can therefore be
considered as consisting of two stages: chemical dissolution
of oxide films by hydrofluoric acid and their formation due to
reduction of HNO3.
TABLE 4. Instability Constants of Complex Compounds
Instability
constants
A1F6 ~ A1F-+F-
0,37
1F4.f A1F3+F-
7,2.10-2
A1F3 A1F2 +F-
1,5.10-4
A1F2 A1F2+-}- F-
5,0.10-6
A1F2+ F A13t+F-
4,8.10
From an analysis of the material given it becomes quite
evident that the electrochemical protection of stainless steels
in HNO3 solutions with additions of HF is not possible since in
these media steels corrode rapidly even from the passive state.
For these aggressive media the choice of structural materials
with minimum solubility of the passive oxide films is therefore
the main problem.
However, we should bear in mind that under the condi-
tions used to dissolve fuel elements the corrosive activity of
HNO3 solutions with HF additions can decrease considerably
in time. This may be due to a reduction in the HNO3 con-
centration and due to the accumulation of metal ions in the
solution (part of the composition of the fuel elements), able
to form stable complex compounds with the fluorine ions. These metals can be all the elements listed below, ar-
ranged in order of increasing stability of their complex compounds with the fluorine ion: iron, beryllium, aluminum,
plutonium, thorium, and zirconium [27].
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. Figure 15 shows results characterizing the corrosion rate
of.18-8 steel with titanium in an 8-M solution of HNO3 with
varying content of HF, as a function of the ratio of the molar
concentrations of aluminum and zirconium nitrates to fluorine.
JCI VCU III LI115 LGbC 14 UUC LU 4 LCUUULIUI1 III LII nr L:UIIL eIILL4-
tion. It is a well-known fact that Al 3+ ions form a series of
bility constants of which fall with increase in the Al/F ratio.
of A13+ ions in the solution more stable complex compounds of
aluminum with fluorine can exist; this leads to a reduction in
the concentration of free HF in the solution. When the limit-
ing ratio Al/F is reached in the solution there will evidently
1,0 only be one compound AlF2+ with a minimum instability con-
stant for the system Ala+-F-. A further increase in the alum-
1,2 inum concentration in the solution should lead to a smaller re-
duction in the HF concentration, due to displacement of equi-
librium of the last reaction to the left (see Table 4). For an
0 ? 4 6 8 48 SO creases more slowly. Similarly, we can explain the reduction
If, g/m2 ? h in corrosion when zirconium nitrate is added to the solution.
Fig. 17. Dependence of the corrosion rate of Since complex compounds of zirconium with fluorine are more
Kh23N27M3D3T steel in a boiling solution of stable than aluminum compounds, the zirconium naturally slows
6 M H2SO4 on the potential. down the corrosion process more effectively (curves 3 and 4 of
Fig. 15). We should expect that ions of the type Al 3+ appear-
ing in the solution due to dissolution of the fuel elements should
be more active in forming complexes with the fluorine ions than the Al 3+ ions from the added nitrate salt, i.e., slow
down the corrosion of stainless steels more effectively.
It therefore follows that in the dissolution of fuel elements the corrosive effect of HNO3 solutions with addi-
tions of fluorides with respect to structural materials will depend to a considerable extent on the presence, rate of
accumulation and final concentration in the solution of ions which form stable complex compounds with the fluor-
ine ions.
Sulfuric Acid Solutions*
To dissolve the cans of stainless steel fuel elements 4-6 M boiling solutions of sulfuric acid are used [1].
Kh23N27M3D3T stainless steels are used to construct the complex chemical apparatus and feed system needed for
operation with H2SO4 solution [28, 291. The corrosion rate of these steels in H2SO4 solutions with a concentration up
to 10 M does not exceed 0.1 g/m2 ? It at temperatures up to 100?C. However, in boiling H2SO4 solutions the corro-
sion rate of steel increases considerably (Fig. 16) and in 6 M acid it is 2-3 g/m2, It. The stationary potential for the
corrosion of steel in boiling 6 M H2SO4 corresponds to the region of the active state and is equal to +0.07 V(Fig. 17).
It follows from Fig. 17 that the corrosion rate should decrease on contact between Kh23N27M3D3T steel with
18-8 steel which is dissolving at?a more negative potential. In fact, in this case the corrosion rate ofKh23N27M3D3T
steel decreases to 0.2 g/m2 ? h, and the potential reduces to -0.05 V, i.e., there is cathodic electrochemical pro-
tection of the structural material. The main breakdown of reactor-dissolvers made from the considered structural
material will evidently occur at the start of the process until there is intensive dissolution of the stainless steel fuel
element cans and after completion of the process of dissolution. At these stages of the technological process the
corrosion of the material of the reactor-dissolver can evidently slow down. For this purpose it is sufficient to add to
the boiling H2SO4 solution some oxidizing agent which can displace the potential of the structural material of the
reactor to the region of the stable passive state.,,.- Experiments show that the addition of 0.2 g/liter of Fe 3+ ions to
boiling 6 M H2SO4 solutions displaces the potential of Kh23N27M3D3T steel to 0.9 V and the corrosion rate becomes
0.2 g/m2 ? h.
* The experimental part was performed by N. A. Bozin.
Contact with 18-8 steel
I I
H
I
I
I
i f
S?added Fe
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We have analyzed experimental data on the corrosive activity of fuel element solvents with respect to struc-
tural materials, using modem ideas on the dependence of the corrosion rate of metals and alloys on the potential;
the following general conclusions were reached:
1. The acceleration of the corrosion of 18-8 steels in boiling (8-14 M) HNO9 solutions is connected with the
disturbance in their passive state and dissolution according to a superpassivation mechanism. The corrosion of steels
in boiling 10-14 M HNO3 solutions proceeds with preferential cathodic control. The possibility has been established
of a sharp increase in the corrosion rate of steels in dilute HN03 solutions when there is contact with electronegative
metals.
2. Monel metal, the most corrosion-resistant structural metal in HF solutions, breaks up in the vapor phase at
rates which care an order higher than these inside the solution. This phenomenon is due to the fact that the corro-
sion of monel metal proceeds with oxygen depolarization with preferential cathodic control. The corrosion of monel
metal is accompanied by cracking, having a specific character.
3. Small additions of. fluorides to HNO3 solutions sharply reduce the corrosion resistance of stainless steels.
The degree of corrosiveness of fluoride additions is a function of the hydrogen ion concentration and appears over
a wide region of potentials. The catalytic accelerating action of fluoride additions on the corrosion of stainless
steels in HNO3 solutions amounts to the facilitation of the anodic process due to dissolution of the passivating films
by hydrofluoric acid. We have shown that the retardation of the corrosion of steels by A13+ ions is due to a reduction
in the concentration of free HF, due to the fluorine ions being combined into stable complex compounds.
4. We have shown the possibility of reducing the rate of corrosion of Kh23N27M3D3T steel in boiling H2SO4
solutions by cathodic protection and the introduction of additions of oxidizing agents to the solution, displacing the
potential of the steel to the region of the stable passive state.
1. F. Culler and R. Blanco, Report No. 1930 presented by the USA to the International Conference on the Peace-
ful Uses of Atomic Energy, Geneva (1955).
2. K. F. Bonhoeffer, In: Transactions of the Fourth Conference on Electrochemistry [in Russian], Moscow, Izd.
AN SSSR, p. 579 (1959).
3. S. Edeleanu, Nature, 173, 739 (1954).
4. Ya. M. Kolotyrkin, N. Ya. Bunk, and V. M. Knyazheva, In: Transactions of the Fourth Conference on Electro-
chemistry [in Russian], Moscow, Izd. AN SSSR, p. 594 (1959).
5. A. M. Sukhotin, In: Transactions of the Fourth Conference on Electrochemistry [in Russian], Moscow, Izd.
AN SSSR, p. 621 (1959).
6. Chemical Processes and Equipment, Reports of the United States Atomic Energy Commission [Russian trans-
lation], Moscow, Izd. inostr. lit. (1956).
7. J. Biinger, Werkstoffe and Korrosion, 9, 747 (1958).
8. J. Truman, J. Appl. Chem., 4, 273 (1954).
9. A. B. McIntosh, Chem. and Ind., No. 22, 687 (1957).
10. W. Walker, Werkstoff and Korrosion, 10, 113 (1959); 11, 563 (1960).
11. M. M. Kurtepov and G. V. Akimov, Dokl. AN SSSR, 87, 93; 795; 625 (1952).
12. M. M. Kurtepov and A. S. Gryaznova, Dokl. AN SSSR, 135, 899 (1960).
13. K. Vetter, Z. phys. Chem., 194, 199 (1950).
14. A. M. Sukhotin, Zh. neorgan. khim., No. 8, 1277 (1959).
15. G. V. Akimov, The Theory and Methods of Investigation into the Corrosion of Metals [in Russian], Moscow;
Izd. AN SSSR (1945).
16. N. D. Tomashov, Theory of Corrosion and Protection of Metals [in Russian], Moscow, Izd. AN SSSR (1959).
17. E. N. Mirolyubov, M. M. Kurtepov, and N. D. Tomashov, Izv. AN SSSR, Otd. khim. nauk., No. 7, 1178 (1960).
18. N. D. Tomashov, M. M. Kurtepov, and E. N. Mirolyubov, Zh. fiz. khim., 32, 904 (1958).
19. E. N. Mirolyubov, M. M. Kurtepov, and N. D. Tomashov, Izv. AN SSSR, Otd. khim. nauk., No. 6, 1015(1960).
20. E. N. Mirolyubov, M. M. Kurtepov, and N. D. Tomashov, Izv. AN SSSR, Ord. khim. nauk., No. 6, 1015 (1960).?
21. B. Morton, Corrosion, 1, 228 (1945).
22. M. Schussler, Industr. and Engng. Chem., 47, 135 (1955).
23. H. Copson and G. Cheng, Corrosion, 12, 647 (1956).
* [19] and [20] are identical and appear this way in the Russian [Publisher's note].
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24. I. L. Rozenfel'd, Inhibitors of the Corrosion of Metals in Neutral Media [in Russian], Moscow, Izd. AN SSSR
(1954).
25. Nucl. Sci. Abstrs., 13, 8609, 8632, 9842, 19983 (1959); 14, 4381, 4385, 5261, 9732 (1960).
26. I. Oknin, Zh. prikl. khim., 24, 167 (1951).
27. K. B. Yatsimirskii and V. P. Vasil'ev, Instability Constants of Complex Compounds [in Russian], Moscow. Izd.
AN SSSR (1959).
28. E. V. Zotova, Stal', No. 6, 552 (1958).
29. V. V. Andreeva and T. P. Stepanova, Investigations into Stainless Steels [in Russian], Moscow, Izd. AN SSSR,
p. 92 (1957).
All abbreviations of periodicals in the above bibliography are letter-by-letter transliter-
ations of the abbreviations as given in the original Russian journal. Some or all of this peri-
odical literature may well be available in English translation. A complete list of the cover-to-
cover English translations appears at the back of this issue.
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RADIATION DOSIMETERS BASED ON THERMOLUMINESCENCE
MEASUREMENTS IN ALUMINUM PHOSPHATE GLASS (IKS DOSIMETERS)
I. A. Bochvar, A. A. Vasil'eva, I. B. Keirim-Markus,
T. I. Prosina, Z. M. Syritskaya, and V. V. Yakubik
Translated from Atomnaya Energiya,'Vol. 15, No. 1,
pp. 48-52, July, 1963
Original article submitted May 19, 1962
Glass dosimeters useful in beta-gamma dosimetry, slow neutron dosimetry, and the dosimetry of
high-energy charged particles in the 0.02 to (1-2). 106 rad range have been developed. The dosi-
meters are capable of storing and retaining information for an unusually long interval (as long as
a month in a 150?C environment). These glasses are not excited by daylight, but daylight does
exert a deexcitation effect: 26 to 38% of the stored light sum is dissipated by deexcitation in a
period of 40 days.
The effective atomic number of the optimum glass recipes is 11 to 13. A filter of 0.6 mm
Sn+ 0.5 mm Al helps counteract the "hardness variation" in the range from 40 keV on higher, within
an error of f 20%. The glass dosimeters are usable repeatably.
Suggestions have been made on repeated occasions to take advantage of the thermoluminescence of crystal
-phosphors in dosimetry (such phosphors as CaSO4-Mn [1]; CaSO4-Sm [2]; CaF2-Mn, LiF [3] have been recom-
mended). The phenomenon of radiophotoluminescence [4] and browning' of glass in response to a radiation exposure
[5] are used to advantage in glass dosimeters.
Temperature, ?C
285 355 370 375
200 300
Time, sec
Fig. 1. Thermal deexcitation curves for 7 x 30 x 30
mm glass specimens exposed to 0.1 r Co60 gamma
radiation: 1) 50-26 glass; 2) 340-3 glass; 3) 20-3 glass;
4) emission by heating unit.
10-2 10-' 100 10 10 1010" 10 10 107Ij, rad
Fig. 2. Gamma dosage de-
pendence of peak thermo-
luminescent brightness of
various glasses (Co60 gammas).
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'fl '%
80
?
70
A,%
90
80
70
60
S0
40
30
20 25 30
b
Time, days
This paper describes thermoluminescent dosimeters
made of aluminum phosphate glass [6]. The method ap-
plied is based on the fact that the energy of the ionizing
radiations absorbed by the glass is stored in the glass in the
form of a luminescence light sum, which is reemitted when
the glass is heated, and may be recorded. Glass compositions
studied included: RxO' P205-A1203; 3P205, where RxO is one
of the oxides of Li, Na, K, Rb, Cs, Be, Mg, Ca, Zn, Sr, Cd,
Ba, or Pb. Multicomponent glasses containing oxides of two
or more elements belonging to groups I and II in the periodic
table, as well as Si02, are also being studied. Activators in
use are Cr, Mn, Fe, Co, Ni, Cu, Ag, Sn, Sb, Ce, Pr, Nd, Sm,
Pb, Bi, and U. Optimum compositions activated by Mn02
(0.1 wt. %) were selected. These are glasses made with partial
utilization of raw materials in the form of sulfates: 5?-26-
MgO ? P2O5-A12O3. 3P205; 34?-3-SrO P205-A1203 3P205;
2? s-Li20 ?p205- A1203. 3P205; and 58? t-SrO ?P205- Si02
? P2O5- 2(A1203' 3P205). Wafers 4 x 15 x 15 mm and 7 x 30
x 30 mm were fabricated for the dosimeters. One square
side of the wafers was polished, and the remaining were given
a matte finish. The thermoluminescent emission was meas-
ured in a special heating unit [7] by means of a FEU-29 pho-
Fig. 3. Variation in stored light sum (A) as a function tomultiplier tube; the thermal deexcitation curves were meas-
of shelf time (a) 5?-26 glass; b) 34?-3 glass]. ured with an automatic recorder. Inspection of Fig. 1 im-
mediately reveals the fact that heating took place at an un-
even rate as dc current was passed through the heater. The
temperature emission of the furnace, which governs the senstivity limit, depends on the current.
0 0,05 0,10 0,15 0,20 0,25 0 0,05 0,10 0,15 0,20 0,25 0 0,05 0,10 0,15 0,20 E, MeV
?
?
?
100
C
a
?
?
150?C
S 10 15 20 25 39 35 40 45
a Time, days
? ?
8
0
0
-
-
150?C
r
100?C
Fig. 4. Hardness variation of gamma radiation (F) for specimens of 5?-26 glass 4 mm thick (figures on
curves indicate filter thickness, in mm): ) filter with 0.5 mm aluminum substrate;
. . . . . . . . . . ) unbacked filter.
The emission of the glasses is in the orange region, and is apparently due to the Mn2+ ion in a position with
coordination number 6 [8]. The energy yield of the light sum amounts to 2-5% in the glasses. As we see from Figs.
1 and 2, the 7 x 30 x 30 mm glass dosimeters are capable of recording doses from 0.02 to (1-2). 106 rad. Hence, the
I
Sn
Pb
T
I
Cu (
-
--,
0
0
0
0,2
0,3
01
0,5
70
0
0 :
-
-
~
0,6
1'0
,
-
---
-
2,5
1721,1
i1~8
0,5
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full range of measurement encompasses eight orders of magnitude. At doses upward of 104 rad, a pronounced colora-
tion of the glasses is observed in pink. and violet colors, and this enables us to determine even larger doses from the
change in optical absorption. Special experiments using glass specimens of different thickness have succeeded in
showing that thermoluminescence saturation at doses _106 rad is not due to increased thermoluminescent absorption
in the glass as a result of browning of the glass.
By comparing our findings with the readings of ferrosulfate chemical dosimeters, we found that the amount
of the light sum stored in the glasses is independent on the dose rate of Co60 gammas up to a level of 25 rad/sec, and
independent of the dose rate of protons of -500 MeV energy up to 400 rad/sec (per pulse) (9].
The glass dosimeters are always ready for service and are capable of storing and retaining information for an
unusually protracted time interval. As we see from Fig. 3, the glasses 5?_6 and 340-9 are capable of measuring doses
over a month or longer, with the introduction of appropriate corrections, even in a 150?C environment. In one of the
experiments, dosimeters of this type were issued to personnel present for 122 days in a field of gamma radiation with
little variation in dose rate. The dosimeter readings upon conclusion of the experiment averaged out at 98.5i 2.5%
of the true value. Tentative calculations reveal that the energy depth of electron traps in the glasses is about 2 eV,
and that at ordinary temperatures the light sum in these should be retained for centuries.
5)
.0
0
x
11 111Z 1 1 11 1111N I-TIT
1-+itt% .....I....I...1111111 11 I 1 Illy
a 10 2 5 f0" 2 5 fp-' 2 5 IT
Mn02 concentration, wt.
Fig. 5. Peak thermoluminescent brightness of MgO glasses as
a function of Mn02 concentration: ... (?) A12O3. 3P205; -?-
(X) 3(A1203. 3P205)-MgO ? P2O5; ---(0) A12O3. 3P2O5-3(MgO
P2O5); (p) 50-26, - .. - ..- (0) Li2O ? P205- MgO
P2O5- SrO ? P2O5 S'02 . P2O5- 4(A 1203. 3P205).
The broad range of the measurements and the unlimited information storage time, combined with the me-
chanical and chemical stability, render thermoluminescent glases ideal memory units.
The glasses remain virtually unaffected by daylight. To check the degrading effect of daylight, a batch of
exposed glasses, of recipes 50-26, 580-t, and 340-3, were left out in the open over a 40 day period. A comparison of
the peaks on the thermoluminescence degradation curves for the glasses exposed in the open and for glasses wrapped
in black paper showed that the peaks on the curves were reduced by the daylight exposure by as much as 36, 38, and
2616, respectively, for the three types tested. The degrading effect of daylight is quite modest, as we see, but shield-
ing against daylight would be required in the case of prolonged exposures.
The sensitivity of personnel glass dosimeters (IKS dosimeters) to various types of ionizing radiations has been
investigated. The hardness variation observed in the recording of gamma radiation is determined, as we know, by
the effective atomic number Zeff, and also by the specimen thickness. Calculations of Zeff for these glasses yielded
values ranging from 11.8 for 20-3 glasses to 18.6 for 340-3 glass. As we see from the calculations, in glasses 4 mm
thick and containing no strontium, the hardness variation does not exceed 350%. Experimental research has aided
in the-selection of a filter to counteract this hardness variation. For 50-26 glasses, a 0.6 mm Sn+ 0.5 mm Al filter
compensates for the hardness variation with an error of ?20% in the 40 keV range and higher (Fig. 4).
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IKS dosimeters and other types of dosimeters were exposed to a flux of 100 to 500 MeV protons at the syn-
chrocyclotron of the Dubna Joint Institute for Nuclear Research. It was found that the sensitivity of the glasses to
a tissue dose of high-energy protons agrees, to, within '10% accuracy, with the sensitivity of the glasses to a dose
of gamma rays, and the glasses are consequently pronounced suitable for use as dosimeters in mixed p-y-emission.
A comparison of the thermoluminescence degradation curves of glasses irradiated by thin Pu239 applicators
and Co" gamma photons aided in determining the a/S ratio of the light sum yield, which came to 16-18% for the
50-2G, 340-3, and 580-t glasses, and to 3-7% for the 20-3 glasses and for other glasses containing Li2O. The relative
sensitivity to'products of the Li7(n, (x)T3 reaction proved to be even higher. It was found that the relative sensitivity
to thermal neutrons as compared to the sensitivity to gamma rays is proportional to the lithium content in the com-
position of the glasses. The energy yield of the light sum in response to bombarding by thermal neutrons is '50%
of the value obtained in response to a gamma exposure. Assuming the a/S ratio not to be in excess of 7%6 in the
case of 2.7 MeV alpha particles formed in a nuclear reaction, then the energy yield for tritons of roughly 3 MeV
energy formed simultaneously (and consequently likewise for protons of -1 MeV energy) will exceed 90% of the
gamma yield. We may assume then, on the basis of already available data, that the dependence of IKS personnel
dosimeter readings on linear energy losses of charged particles will be weaker than in the case of organic scintilla-
tors, but still weaker in organic crystals of types NaI (T1) and CsI (T1) [9].
The light sum stored by 20-3 glasses irradiated by thermal neutrons turns out to be greater by a factor of ten
than when irradiated by the same tissue dose of gamma radiation (expressed in rems). Consequently, 20-3 glasses
are attractive for use in determining the dose contribution of slow neutrons against a.background of intense gamma
radiation. Even more suitable for this application are the 30-5 glasses which contain 1.5 times more lithium. A
simple calculation reveals that glasses containing Li2O in amounts of about 1 wt. %are capable of directly measuring
a mixed dose of gammas and thermal neutrons. All of the glasses studied here are virtually insensitive to fast neu-
trons, as we see from calculations of absorbed dose and from direct measurements.
The optimum glass recipes arenot critical. As we see from an example of MgO glasses (Fig. 5), the thermo-
luminescent brightness drops to one-half as the fraction of MgO in the basic composition of the glass varies by afac-
tor of two, and as the Mn02 concentration varies by over one order of magnitude.
Specimens of glass exhibit excellent reproducibility when made in quartz crucibles with stirring of the melt.
Fifty dosimeters produced in a single laboratory-bench operation differed by not more than 15% in the calibration,
and this is commensurate with the accuracy attainable in the measurements.
IKS personnel dosimeters can be used repeatedly. Measurements repeated 50 times with 50-86 and 340-3 glasses
failed to reveal any changes in the thermoluminescence degradation curves. Several specimens of glass have been
in serivce for over three years, and no deterioration of the calibration has been detected.
Some distinct glass compositions containing Li2O yielded poorly reproducible readings in repeated measure-
ments, and this is apparently accounted for by the low softening point of those glasses. It is quite possible that ir-
reversible ionic or chemical processes affecting the emission yield take place at an appreciable rate in the glasses
even at the temperatures at which the thermoluminescence degradation curves were measured.
Five to seven minutes were spent in the laboratory measurements to plot the thermoluminescence degradation
curves. At the present time, new heaters are being developed to aid in successfully shortening the measurement time
to 2 min with no losses in sensitivity.
The broad range of measurable dose levels and the protracted retention of information make it possible to
consider glass dosimeters for use in the practical solution of quite a few problems. The method is well suited to per-
sonnel dosimetry of S-y-radiation, slow neutrons, and high-energy charged particles with a weekly-quarterly ex-
posure cycle. IKS personnel dosimeters may apparently be used to record a radiation dose obtained over the entire
service life of the dosimeter, as well as for individual personnel dosimetry in emergency and overhaul or mainten-
ance operations. They may prove useful as dosimetric monitors in x-ray therapy and in some other areas of appli-
cations of radiation effects, such as sterilization of potatoes, disinfection, etc. Thanks to its properties, the method
is feasible as a tool of scientific experimentation in the study of dose fields under extreme conditions, i.e., very
minute doses, including doses of background radiation, as well as for the study of a very wide range of doses under
high temperature conditions, in a corrosive medium, etc.
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LITERATURE CITED
1. W. Kossel, U. Mayer, and H. Wolf, Naturwissenschaften, 41, 209 (1954); B. M. Nosenko, L. S. Revzin, and
V. L. Yaskolko, Zhur. tekhn. fiz., 26, 2046 (1956); V. A. Arkhangel'skaya, et al., JAE,8, 559 (1960).
2. H. Peter, Atomkernenergie, 5, 453 (1960).
3. D. Patterson and H. Friedman, J. Opt. Soc. America, 47, 1136 (1957); R. Ginther and R. Kirk, J. Electrochem:
Soc.. 104, 365 (1957).
4. J. Schulman, et al., Nucleonics, 11, 52 (1953).
5. J. Schulman, et al., Nucleonics, 13, 30 (1955); N. Kreidl and G. Blair, Nucleonics, 14, 56, 82 (1956); 17, 58
(1959).
6. I. B. Keirim-Markus, Z. M. Syritskaya, and V. V. Yakubik, Steklo. Byull. Gos. inst. stekla, No. 2 (111), 77
(1961); I. A. Bochvar, et al., Ibid., No. 2 (1963).
7. I. A. Bochvar and I. B. Keirim-Markus, Pribory i tekhnika 6ksperimenta, No. 6, 139 (1961).
8. S. Linwood and N. Weyl, J. Opt. Soc. America, 32, 443 (1942).
9. Radiation dosimetry, Edited by Hine and Brownell, Academic Press, N.Y. (1956).
All abbreviations of periodicals in the above bibliography are letter-by-letter transliter-
ations of the abbreviations as given in the original Russian journal. Some or all of this peri-
odical literature may well be available in English translation. A complete list of the cover-to-
cover English translations appears at the back of this issue.
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MONITORING IONIZING RADIATIONS RESULTING
FROM NITROGEN REACTIONS
M. T. Dmitriev
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 52-59, July, 1963
Original article submitted October 30, 1961
Problems of monitoring ionizing radiations and neutrons from nitrogen reactions taking place on ir-
radiation of air, nitrogen-oxygen mixtures, nitrogen oxides, or water containing dissolved air and
during capture of neutrons by nitrogen nuclei are discussed. Nitrogen-oxygen and nitrogen oxides
ionizing-radiation and thermal neutron monitors are proposed on the basis of the investigated ra-
diation-chemical effects. The lower limit of measurement of radiation dosage is 1 rad, and that
of an integral neutral flux is 109 neutrons/cm2. Use of the appropriate procedure makes it possible
to reduce these limits. The upper limits of measurement of dosages and neutron fluxes by open-
type monitors are virtually unrestricted. The method makes it possible to carry out dosimetric
measurements from samples of air and water under natural conditions.
The literature contains fairly numerous examples of determination of average and high doses of ionizing ra-
diations from various physicochemical processes taking place under the effect of radiation in phosphors, glasses, aque-
ous solutions of inorganic compounds, carbohydrates and other substances. Our method of monitoring ionizing ra-
diations from various nitrogen reactions is included in this type of monitors. Nitrogen monitors make it possible to
determine doses by y-radiation, electrons, protons and other types of ionizing radiations (starting at 1 rad) and in-
tegral neutron fluxes (starting at 109 neutrons/cm2). The most essential difference between monitoring from nitro-
gen reactions and other chemical monitoring methods is the possibility of direct determination of the amounts of
absorbed energy by means of air samples taken from radiation apparatus, industrial plant or the atmosphere, andsam-
ples of water from soil or lakes. Futher, the monitor may be filled with, say, air; this is an undoubted advantage
whether in the laboratory or in field work. Monitors based on nitrogen radiation reactions may also be employed
in radiobiological investigations.
TABLE 1. Energy Yield of NO2 Formation Reaction in Air at Atmospheric
Pressure in Relation to the Type of Ionizing Radiation (from data in [1-5])
Temp., ?C
NO2 yield,
mol/100 eV
17.5
1.4
30
1.45
150
2.45
15
1.35
45
1.5
65
1.6
145
2.4
Protons
30
1.5
Ions and electrons
25
1.4
Nuclear reaction radiation
30
1.55
The same
49
1.8
140
2.5 ?
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Nitrogen-oxygen system. In [1] I investigated the effect of ionizing radiations on nitrogen-oxygen mixtures,
particularly air. It was found that the primary elemental process leading to active nitrogen reactions is ionization
of the nitrogen molecule. Reaction of nitrogen with oxygen commences, and is accelerated, at electron energies
corresponding to formation of molecular and atomic nitrogen ions. The reaction rate is proportional to the value
of nitrogen ionization. The following reactions may consist either of direct chemical reaction between a nitrogen
molecular ion and an oxygen molecule, or reaction of the dissociation products of a molecular ion (an atom and
atomic ion) with oxygen. Furthermore, recombination and recharging of ions play a considerable role in the reac-
tion. As a result of ionization processes and the subsequent radiation-chemical reactions, primarily NO, NO2, and
N20 are formed. Other, unstable nitrogen oxides, which are converted to NO2 during analysis, are also formed. If
molecular oxygen remains in the irradiated mixture (which is nearly always the case) NO is converted to N02-
Therefore, the principal radiolysis products of air are NO2 and N20. Formation of NO2, the amount of which may be
readily determined by simple methods, is of maximum interest.
1 2.10
Dose, rad
Fig. 1. Relation between NO2 concentration and
fast-electron and y -radiation dose. Pressure 1
arm; temperature 20?C; composition of the mix-
ture: 0) 50% N2+ 50% 02; i) 70% N2+ 30% 02;
?) air; V) 90% N2+ 101 02.
61 50 100 150
4
1 2 3
Fig. 2. Relation between the NO2
energy yield and pressure. Tempera-
ture 20?C; composition of the mixture:
1) 90% N2+ 10% 02; 2) air; 3) 50% N2
+ 50% 02; 4) air.
Table 1 gives the energy yields of NO2 formation by the action of various ionizing radiations on air at at-
mospheric pressure. It may be seen that the energy yield of NO2 formation is virtually independent of the type of
ionizing radiation and therefore the ionization density; this is an undoubted advantage in monitoring a mixed ra-
diation field. -Approximately the same energy yields (related to the same temperature) are obtained from the ac-
tion of electrons and y-radiation and from irradiation of air by fission fragments [6]. Roughly the same results were
also found for electric discharges in air [2, 3].
The values in Table 1 were obtained under different conditions and differing degrees of accuracy and can
therefore only serve for a rough assessment.
Measurements were carried out to improve the accuracy of the NO2 energy yields in air at atmospheric pres-
sure under the effect of Co 60 y -radiation and 0.2 MeV electrons. The NO2 contents were determined by the spec-
trophotocolorimetric method, the absorbed irradiation energies were measured in a calorimeter with distilled water,
described briefly in [4]. In particular, the following results (accuracy 1-3%) were obtained:
Temperature, ?C 0 10 15 20 25 30
NO2 molecule/100 eV 1.35 1.38 1.39 1.41 1.43 1.46
These values may be employed in radiation-monitoring measurements, irrespective of the type of ionizing. radiation.
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It was noted above that the NO2 formation reaction
is directly related to ionization processes. A specific num-
ber of NO2 molecules formed in this process corresponds to
a particular number of the ions initially formed in air.
Measurement of the concentration of ions formed in air is
obviously only possible during the radiation process be-
cause most of the ions are neutralized as a result of re-
combination processes immediately after radiation has
ceased. But the NO2 molecules formed during ionization
of air and subsequent reactions of the ions remain in the
air for an indefinite period after radiation has ended. There-
fore, the number of .ions formed during radiation, but sub-
sequently recombined, may be determined reliably from
the concentration of the NO2 method.
too
Temperature, ?C
The action of the monitor based on radiation reac-
tions. of nitrogen ions and dissociation products of the latter
in air is based on this effect. For a nitrogen-oxygen mon-
itor of ionizing radiation (or merely of a sample of free
air), radiation of 1 roentgen produces 9.15. 108 molecules
of NO2 in 1 cm3 of air (at 0?C and 760 mm Hg) (based on
Fig. 3. Relation between the NO2 energy yield and
temperature for air._ Pressure, atm: O.) 150; I) 10;
i) 0.1; ^) 5; V) 1.
a mean energy of 32.5 eV
in air at 760 mm Hg correspond to a dose of 1
10-8 Wt. 616 at 20?C.
of one ion pair in air). The following NO2 concentrations formed
rad: 0.64' 10-8 wt. 016 at.0?C, 0.66' 10-8 wt. jo at 15?C, and 0.67
Apart from the absorbed radiation energy, the concentration of the NO2 formed also depends on the com-
position of the mixture, temperature,and pressure. Figures 1-3 give data on the relation between the NO2 concen-
tration and these factors. When air samples taken at pressures other than atmospheric (e.g., at great heights) or at
high temperatures are analyzed, appropriate corrections must be made for the relation between energy yield and
these factors. Corrections must also be made if the monitor is filled with a nitrogen-oxygen mixture of different
composition to air.
Figure 1 gives the relation between NO2 concentration and the absorbed dose for mixtures of different com-
position. This shows that in the initial section, the NO2 concentration is directly proportional to the dose up to
^-1.5.109 rad:
[NO2] = kE,
where [NO2] is the NO2 concentration, wt. 1o; E is the absorbed dose, rad; k is the proportionality coefficient.
At 20?C and 1 atm the values of the coefficient k ? 109 in relation to the mixture composition are as follows:
Air
5.12
90% N2+ 10% 02
2.86
70% N2+ 30cJo 02
6.72
50% N2+ 50% 02
7.98
15% N2+ 85% O2
4.08
According to [1, 4, 51, for other nitrogen-oxygen mixtures irradiated at 20?C at atmospheric pressure the co-
efficient k may be obtained from the equation
k = 32,On (1- n) ? 10-9,
where n is the mole fraction of nitrogen in the gas mixture.
Equation (1) is not satisfied at electron doses higher than 1.5' 109 rad, but calculations may still be made up
to 2.5. 109 rad from the relations given in Fig. 1. For electrons and y-radiation, above 2.5. 109 rad, the NO2 con-
centration is independent of the value of E because a stationary state in which the decomposition rate of NO2isequal
to its formation rate is established in the gas mixture.
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TABLE 2. Values of the Coefficient k (x 109) in Rela- In [7] it was established that the NO2 stationary
tion to Pressure at 20?C concentration depends on the ionization density be-
cause the efficiency of NO2 decomposition depends on
Gas mixture, Pressure, atm decomposition by
the latter. The energy yield of NO2
fission fragments is several times less than for decom-
0,1 0,5 1 10 20 100 150
position by electrons and y-radiation. Therefore the
stationary concentration of NO2 by fission fragments is
Air 8,6 6,3 5,1 14,4 15,7 19,2 20,4.
several times higher than for irradiation by electrons.
z -I 10 02 a,8 3,5 2,9 11,7 14,6 17,9 18,9
02 13,3 9,8 8,0 17,1 17,4 21,1 22,5
50N2+50 In air the stationary concentration is 6 vol. % for the
30N,,+70 ,+-70 02 11,2 8,3 6,7 16,4 16,7 20,5 21,7
latter [1] and 20.3% for fission fragments [8]; in a 1: 1
mixture these figures are 12% and 43.7%, respectively.
TABLE 3. Values of k (x 109) for Different Air Pres- From an analysis of the shape of the curve of NO2 con-
sures in Relation to Temperature centration versus the dose (Fig. 1), it may be concluded
Air
Tempe
rature,
?C
pressure
atm
f 0
20
30
70
100
150
200
1
4,9
5,1
5,3
6,0
6,9
9,6
11,9
0,1
7,7
8,6
8,9
10,6
12,8
17,2
20,0
5
10,0
10,4
10,5
10,8
11,1
12,0
128
10
14,1
14,4
14,7
14,9
15,4
16,2
16,8
150
20,2
20,4
20,5
20,8
21,0
21,3
21,5
that in the case of fission fragments Eq. (1) will be satis-
fied up to doses of 7. 109 rad.
Figure 2 gives the relation between the NO2 energy
yield and pressure for mixtures of different composition.
With an increase in pressure above 1 atm the NO2 energy
yield increases, but does not exceed 6 mol NO2/100 eV.
The energy yield also increases to some extent if the
pressure falls below 1 atm. The minimum values of the
energy yield at a pressure slightly above 1 atm are re-
lated to the maximum of ion recombination efficiency
[1]. Table 2 gives some values of the coefficient k in
relation to pressure.
Figure 3 gives the relation between NO2 energy yield and temperature in the range 0-200?C. It may be seen
that the yields increase with temperature, but with increasing pressure this increase is less marked. Table 3 gives
some values of k in relation to temperature for air at different temperatures.
With an increase in temperature above 200?C the NO2 energy yield falls, one of the causes being thermal de-
composition of NO2 to NO and oxygen. At the same time the energy yield of radiation decomposition for NO by
electrons and y-radiation is 7.1 times greater than for NO2 [7]. This is due to a slight increase in the NO and NO2
formation yield in air > 200?C. Further, it was found that NO molecules formed by irradiation of nitrogen-oxygen
mixtures, and present in different excited states, transfer their excitation energy to the gas molecules in the form
of kinetic energy and light radiation, and to other molecules during ion recombination and charge transfer processes.
With a considerable increase in energy the excited molecules become unstable. Some of them decompose without
ever reaching a normal state. The relative number of decomposed molecules depends on the temperature.
The following values of the NO2 formation energy yield at high temperatures in air (atmospheric pressure) may
be taken as correct to 5-10%a
Temperature, ?C
0
200
300
500
750
NO2 molecules/100 eV
1.35
3.3
2.7
1.6
0.7
The N20 formation reaction may also be used for monitoring, but in this case the analytical procedure is some-
what more complicated. The N2O energy yield in air increases with pressure. The following results were obtained
at 20?C:
Pressure, atm
1
5
10
25
50
100
150
N2O molecules/100 eV
0.62
1.2
1.8
2.1
2.9
3.1
3.2
Asa radiation monitor N2O is the best form to employ when taking samples of free air because NO2 is not sufficiently
stable under natural conditions.
In liquid nitrogen-oxygen mixtures (at about -183?C) at a 1: 1 N2: 02 ratio, the NO2 yield is 1.2 while that of
N20 is 0.8 mol/100 eV (the values for liquid air are 1.1 and 0.7, respectively).
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In addition to. nitrogen oxides, ozone is formed in nitrogen-oxygen mixtures. The ozone yield in air at 20?C
is about 3.5 mol/100 eV (-'8 mol/100 eV in pure oxygen). In a liquid nitrogen-oxygen mixture (1: 1) the ozone
yield is ^-3 mol/100 eV (in liquid oxygen -5.5 mol/100 eV). The use of the ozone radiation formation reaction for
monitoring is greatly complicated by the instability of ozone at high temperature, by the fact that ozone may de-
compose on metal surfaces and by other factors.
Under natural conditions, with free air sampling, ozone monitoring gives satisfactory results (accuracy up to
10%) with respect to absorbed energy. Formation of deposits greatly reduces the measurement accuracy.
In addition to ionizing radiation monitoring, determination of the ozone concentration in air allows one to
find the absorbed energy of electric discharges. I employed this in my method for forecasting electrical storms of
low probability, which is based on the fact that absorption of discharge energy in air (and therefore the appearance
of high ozone concentrations) occurs mainly 2-3 hours before the storm commences, at the time of cumulus formation.
NO2 formation in nitrogen-oxygen mixtures by ionizing radiations may also be used for measuring neutron
fluxes. As a result of an N14 (n, p)C14 nuclear reaction, irradiation of the nitrogen-oxygen mixture by protons takes
place simultaneously with the formation of radiocarbon. The intensity of proton irradiation can be measured from
the NO2 formation rate [1]. The thermal neutron flux may be determined by means of the following equation:
5,75a vT
1aPG
where f is the neutron flux, neutron/cm2 ? sec; P is the gas pressure in the radiation monitor, mm Hg; T is the tem-
perature, ?K; G is the NO2 energy yield at the given temperature and pressure, mol/100 eV; v is the NO2 formation
rate, mol/cm3 ? sec. The coefficient a (always 2.
Consequently, for economy of computer time the gamma quanta originating from a depth of more than two
mean free paths were assumed to have been absorbed and were left out of consideration.
In the matrix of final results the graduation in angular values was taken through 15?. In energy graduation
the first intervals were taken at 0.03-0.05. and 0.05-0.10 MeV, and thereafter 0.1 MeV intervals were used, apart
from the case E0 = 2.62 MeV, where, starting with E = 0.5 MeV, the interval width was taken as 0.25 MeV.
Results of the Albedo Calculations
Figures la and lb show the curves of the spectral-angular distribution of the intensity of the reflected gamma
radiation I (E0, E, 6)= EN(E0, E, 0) for E0 equal to 1.0 and 2.62 MeV, normalized to primary radiation fluxes of unity.
From an analysis of the calculation results the following conclusions can be drawn:
1. All the energy distributions for the gamma radiation have a maximum (peak) at E ~ 0.25 MeV, with an
amplitude which decreases almost linearly with the angle of inclination 0, with a slight dip (about 20 units) at 0
=40?. As E0 varies, the relative contribution made by the peak to the albedo and its absolute value vary almost
linearly.'
? Calculations in which the reflection from the upper half-space (homogeneous medium) was taken into considera-
tion indicate that because there is multiple albedo, contributing chiefly in the soft region of the spectrum, the po-
sition of the peak is displaced to E =0.1 MeV, in accordance with the data obtained by the method of moments[7].
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As the angle 0 increases, harder quanta appear in the reflected radiation, so that a second maximum (peak)
is formed, primarily caused by the singly scattered quanta and having an amplitude practically independent of '0.
The upper energy limit of the peak corresponds to the maximum possible energy of singly. scattered gamma quanta
in that direction.
0 -1S?
15.3 ?
30,4
145-
60
75-90?
0,8 1,0
E, MeV
0,01
2,62
E, MeV
Fig. 1. Spectral-angular distribution of the intensity of reflected gamma radiation from an isotropic
point source, with Ep equal to: a) 1 MeV; b) 2.62 MeV.
I (E,
10B,H
2 2 H=0,5
0-30?
5 30-60?
3 60-90?
2 0 / - 2,2 ;MeV
b
Fig. 2. Spectral-angular distribution of gamma radiation from an isotropic point source with Ep=1 MeV (a) and 2.62
MeV (b), situated at a depth of 0.5, 1, or 2 mean free paths.
2. We calculated the mean energies of reflected gamma quanta as a function of the observation angle 0, as
well as the mean energies of the total albedo for each E0, that is, the quantities
I (E0, E, 0) (/1; I (E.01 0)..
N (,F. o, 0) d/ N (Lo, 0)
2at I (EO, 0) sill Hit 0 (L'o)
'tt S N (En, 0) sin it (/. H N (E0): '
0-15?
15-30?
30-4
45-60
60-75?
75-90?
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4
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E(E0, e) increases with increasing 8, and the rate of increase is greatest for 0 > 60?. For albedo in the vertical direc-
tion, that is, for 8 00, E(E0, 0) - 0.2 E0.2, and for 0 > 75?, E(E0, 0) c 0.5 Eo -75.
As shown by the calculations, E(E0)= 0.30 Eo, with an accuracy of the order of several percent.
3. The angular distribution of the total number of reflected gamma quanta per unit solid angle N(E0, 8) de-
pends only slightly on the primary energy, and for observation angles 0 < 70?., it may be described with an accuracy
of about 15% by the function
0
ae 75
The angular distribution of the energy flux per unit solid angle I(E0, 8) for 8 < 70? at E0> 2 MeV is close to the iso-
tropic distribution (with a slight drop of about 15% in the region 8 -45?) and tends to a cosinusoidal distribution as
the primary energy decreases.
4. The total albedo with respect to the number of particles in the observed interval of primary energies may
be approximated by the function RN(Eo) = 0.41 - Eo-0'2, and the energy albedo by RE(Eo) = 0.12 ? Eo-o.75The resulting
values agree to within less than 10% with the results of [1].
Point-Source Gamma Radiation Passing Through a Layer
Figure 2 shows the curves of the spectral-angular distribution of the gamma quantum intensity I(E0, E, 8, H) of
an isotropic point source with Eo =1 MeV and 2.62 MeV, placed at a depth of 0.5, 1, or 2 mean free paths. The
curves are normalized to unit source intensity.
From an analysis of similar curves for the set of primary energies and depths we draw the following conclusions:
1. In contrast to the energy distribution of gamma radiation in a homogeneous medium, the spectrum of
quanta passing through a layer thicker than one mean free path has practically no peak in the soft region.
2. The mean energies of scattered gamma quanta E(E0, 8, H) for depths H`< 0.7 increase with increasing angle
8, reaching a value of about 0.5 E0.
For large absorber thicknesses the quantity E(E0, 8, H) varies comparatively little (about 30%) and assumes
maximum values of the order of 0.4 Eo for angles 40? Of, 60?.
3. The angular dependence of the number of scattered quanta per unit solid angle depends only slightly on
the primary energy, and for H> 0.5 it may be described, with an accuracy of about 20%, by a linear function of H
and 0. In particular, if Eo = 1 MeV, for a source with unit activity
4,27-0,111
1-
9U
The angular characteristic of the energy flux for scattered quanta I(E0, 0, H) for H = 0.5 is approximately cosinusoidal.
As H increases, the directionality increases somewhat.
4. The total intensity, both for the number of emitted scattered quanta N(E0, H) and for their energy I(E0, H),
reaches a maximum if the source is located. in the absorber at a depth of H X1/3 from the boundary surface.
5. The ratios of N(E0, H) and I(E0, H) to the primary radiation intensities are of the nature of integal build-up
factors BN(EO, H)-1 and BE(Eo, H)-1; in the depth and energy intervals under consideration they may be approxi-
mated, with an accuracy of about 10-1516, by the functions
BN (Ho, H)-1=BN (Eo)-f 2,95.10 o,a2lf,
13, o,57II,
where R(E0) is the albedo for the corresponding primary radiation.
In conclusion, the author expresses his gratitude to R. M. Kigan for his appraisal of the results obtained, as
well as Z. D. Dobrokhotova and E. N. Goryanina for their help with the calculations.
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1.. M. Berger and D. Raso, Radiation Res., 12, 20 (1960).
2. M. Berger, J. Appl. Phys., 28, 1052 (1957).
3. Yu. A. Kazanskii, Atomnaya 6nergiya, 8, 432 (1960).
4. G. Whyte, Canad. J. Phys., 33, 96 (1955).
5. M. Berger, J. Res. Nat. Bur. Standards, 55, 343 (1955).
6. C. Davisson and R. Evans, Rev. Mod. Phys., 24, 79 (1952).
7. H. Goldstein and I. Wilkins, Calculation of Penetration of Gamma Rays. NYO-3075 (1954).
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THE RATIO OF THE THERMAL NEUTRON FLUX IN WATER
TO THE POWER OF A POINT SOURCE
E. A. Garusov and Yu. V. Petrov
Translated from Atomnaya Energiya, Vol. 15, No. 1,
p. 71, July, 1963
Original article submitted October 13, 1962
The value of the parameter (Dt/W (the ratio of thermal neutron flux to reactor power) for research reactors
was given in [1]. The same report contained a calculation in the age-theory approximation of the maximum value
4)t/W for a point source with no self-absorption in an infinite medium consisting of a number of substances. The
calculations showed that among all the moderators available for practical reactor use, ordinary water yields the
maximum value of 4,t/W. However, as is known, the age-theory approximation cannot be satisfactorily applied to
water. On the other hand, the three-group theory gives much larger values than the age-theory approximation. It
is therefore of interest to find the value of (Dt/W directly from experimental data. Reference [2] gives measurements
for the distribution of a flux of neutrons with energy E=1.46 eV in water from a U235 point fission source. On the
basis of experimental data the maximum ratio of thermal neutron flux to power was calculated. The age-theory
approximation was used for the moderation of neutrons from 1.46 eV to thermal energies. The age value of Lr = 1
cm2 was taken from [ 3]. A variation of +50% in Zr fiintroduces a correction of not more than 5%6 into 4)t/W.
The diffusion length of the thermal neutrons was taken to be 2.73 cm and the diffusion coefficient 0.165 cm.
The space integral of the experimental curve was normalized with respect to the total number of fast neutrons from
U235 fission.
The error in (Dt/W, caused primarily by the experimental error, was f 2516. The values for 4)t/W ? 10-13
(1/cm2 ? sec?mW) obtained by the age-theory approximation, by the three-group theory, and experimentally were
38,* 100, and 80 t 20, respectively.
The authors express their gratitude to A. N. Erykalov for his critique of the results.
1. S. M. Feinberg, et al., Proceedings of the Second International Conference on the Peaceful Uses of Atomic
Energy [Russian translation], Reports of Soviet Scientists, Vol. 2, Moscow, Atomizdat, p. 334 (1958).
2. L. N. Yurova, A. A. Polyakov, and A. A. Ignatov, Atomnaya energiya, 12, 151 (1962).
3. L. M. Barkov and K. I. Mukhin, Atomnaya dnergiya, No. 3, 31 (1956); L. M. Barkov, V. K. Makar'in, and
K. I. Mukhin, Ibid., p. 33.
* The age value to thermal energies was taken to be 28.3 cm2,
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THE EFFECTIVENESS OF A SYSTEM OF ABSORBER RODS ARBITRARILY
DISTRIBUTED IN A REFLECTED REACTOR
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp.71-74, July, 1963
Original article submitted October 15, 1962
In previous studies [1-3] we found the critical conditions and neutron flux distributions for a homogeneousther-
mal-neutron reactor with a system of absorber rods distributed at equal intervals in a ring in the active zone or the
radial reflector.
In the present study we use a two-group approximation to generalize the case to arbitrarily distributed rods
fully inserted into the reactor.
System of Rods in the Reflector of the Reactor. In a cylindrical reactor with a system of rods placed in an
arbitrary manner in a radial reflector, the solution in matrix form for the fast neutron flux q and the thermal neu-
tron flux (P2 will be
wI 1= [ i i2 J [ Mr _I
,JO
TII [ III I
1 ~~ 1111
[ Si f 0 J [ LI1
l
L1 i (xr) 0 Ain cos n(p } L''1n Sin n(p
A11 J J t_ 0 In (,r) ] C A2n cos nT + F2n sin n~
n=0
r In (vr) (C2n cos n(p-FF2,, sin ncp) - K7z (vr) (D,n cos 77(P+ 11?,, sin 11(p)
I In (?r) (Cin cos ncp ; Fill, ,in n(P)1-Kn (?r) (Din COS 17(P-;-III? sin nrp)
m N
Km (vej) i) B2mi C)Sntwi-i-P'Ili .J L1 ( I B1n7.i COS n7 (ili--i _. ~~1n7i S1:11
0 K,0(LQ) 7077 2(O 1
Wi
m-0 i=1
Here N is the number of rods; i is the index number of the rod; r is the distance from the center of the reactor to
some arbitrary point P; pi is the distance from the center of rod number i to some point P; cp and wi are the corre-
sponding azimuth angles (see diagram); S1, S2, S3 are coupling coefficients; I, II are the indices of the active zone
and the reflector, respectively.*
From the fast neutron flux continuity condition and flux density at the boundary between the active zone and
the reflector
d(pr dcp1I
dr V2. dr
02n, 1'2n) = (= l In, E1n) fn _- E. [B2mi~nm (cos it (Pi) 'r- I~2miwnrn (Sill rl(pi, COs n(pi)),
m=0 i=1
m N
(C2n, F20 _ ( lin, 1%'10) (Pn ' [B27nixnm (cos n (Pi, sin lt(pi)~ p2mixnnt (Sin 77(pi, COS n~i))?
M=0 i=1
N
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Here the functions f n, cPn, (Dnm, Xnm will have the same form as the corresponding functions f n, ..., Xnm in [1], if
we take yi = 1 in those functions; anm is written like (Dnm if, instead of the functions rnm and vnm appearing in the
expression for (Pt1m, weintroduce their value with a bar:
rnm = In-tit (vRi) -- In+m (vHi),
vnm = Kn-ni (vRi)-Kn+m (vRi);
Xnm is written in the same way as Xnm if, in the expression for Xnm, the values of rnm, vnm, 4)nm are taken equal
to rnm, vnm, and anm' respectively.
It should be noted that, since we are considering a system of arbitrarily distributed rods, the index nN in the
Bessel function of [1] should be replaced everywhere by E. and Rc and replaced by Ri. In obtaining Eqs. (3) we used
the addition theorem for Km(v, ppi) and the relationships for the constants Din, D2n and Hin, H2n which are obtained
from the boundary values for iPr and q at the reactor surface (cg = (Pg = 0 for r = Req):
W N
(D2n, II2n)_ - (C-2n, P-211) I (yReq `1 bn -i
SrL) K (V Re) - J IB2mirnm (cos n~i sin nTi) TP2mirnm (sin ncpi; cos n(Pi)];
n q
M=O i=1
W N
(Dirt, Ittn) _ -Win, Fin) hnn (? eq (ltlReq) _ `~ -n IBtmibnm (cos ltpi, sin ?Wi) + Ptmibnm (sin ncPi, cos nc)i)]
) J
m=O i=1
whereon=-l for n=0; 8,L=2 for n.,?,I; bnn7=lrt_nt(N?Ri)-In+m(ltRi).
From the thermal neutron flux continuity condition and flux density at the boundary between the active zone
and the reflector
dcl dq lI
T2-a21' dr -
( Vo dr
Co N
(Cin, F'tn) = LJ 21 [(BLmiQnm+B2miAnm) (cos nlpi, sin n(pi) IF (PimiQnm+P2miAnm) (sin 11(pi, COS ntpi)];
M=O i=1
Co N
(A
tn+ [:ln)= 21 [(Bimi Rnm - {-l3 2miTnm) (Cos ncPi+ sin n(pi) T TT (Ptmi R ~-P T )(SIR Lmi, C,OS ,
nm 2nti nm n~i)]
M-_0 i=1
Here the functions Qnm? Rnm are of the same form as the corresponding functions in [1]; Qnm? Rnm are written in
the same way as Qnm. Rnm if instead of the functions bnm, anm we write their value with a bar: bnm and anm
Kn-m (MRi)-Kn+ m (IRi); nm, Tnm are written in the same way as anm. Tnm if instead of Xnm, (Pnm. rnm, vnm+
and Anm we introduce the corresponding functions Xnm? ??? anm?
If we use the boundary conditions. for cgll and (P jI at each of the absorber rods and the corresponding addition
theorems for Bessel functions for pi < Ri, pi < Pis (pi ~ ai), after some transformations we obtain the following equa-
tions:
N m oo ao
{[B imi (glkillnntki+g2ki 9nm.ki -' -
i=t k=0 m=0 n=0
i 6rnk6isLlki+91kf8,gAimhj)+B2mi (giki(Onmki 'i-
-~g2k{nnmki+8mkOisL ti - I 2i.BsiA
2ki A 2mki)d
-F-8si (glkiPimiQimki+g2kiP2miQ2mki)) cos kcoi +
-i- [Ptmi (gtkillnmki+g2kignmki+8mk8isLiki+
i
+8si9lh1Qtmki)+8si (glkiBimiAimki +e202miA2mki)-{
+2mi (giki(Onmki-I-g2k{nnmki+8mk8isLZki+
g2kibs1Q21nki)l sill kwi.}=0,
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Diagram showing the distribution of the rods in the re-
flector of the reactor.
tdi
{IBI)nir2ki?nnthi+B2mi (,2ki'Tnnikt-!-"
i=t k=0 m=0 n=0
smkSisL2di di di
ki-1-fisi, 2kiA2ntlti)+P2nli5si72k1~'mki1COS
IP1mio'2ki?nna41?P2nti (n?2di i- di
h tnmki+bmhsisL2ki i
f bSi,2ki~'-naki)--B211tibsia2kiA2mkil sin kalif =O.
Here the functions Hnmki, gnmki' Wnmki, and
Trnmki;are of the same form as the corresponding func-
tions Hnmk. lrnmk in [1] (Rc is everywhere taken
equal to Ri); the functions Hnmki, gnmki, Wnmki, and
Trnmki are written like Hnmki, ???, Trnmki if instead of
the functions bnk, bnm, Qnm, Rnm, Onm, Tnm, Xnm,
rnk, rnm, and vnk we use the coirresponding value with
a bar; the functions gtki, g2ki d1, Lllc, L2k~1' dl are
expressed like the functions gik, gJ , Ltk, L21'' d in
[1] if the values of a, y, and d in the latter are taken
equal to ai, yi, and di, respectively; Sis =1 for s = i;
Sis = 0 for 5i; Ssi = 0 for s = i and Ssi = 1 for s -~ i; Smk = 1
for m = k and 6mk=0 for m;~ k[at the surface of the rods
the boundary conditions were given in the form
(drPiI/d/Pi) ((PiI)-l= 11
t
(t441idoi) (w")-t =_ -.1
li
el='til.
The functions Atmki, Aimki, Dtmki, and S21mki, are found from the formulas
..K
nnhi=-Z IKnt+-it([Leis)ens(nt(is-;-k~i)-i
-Kill -h (Weis) cos
Ft R Q
Almki -2 - [Kna+h ([Leis) sin (mP,?kPj) -
_Km.-h ([leis) sin (rots--kpi)l;
t21n1ki=- ~k [Kn1+h ([leis) sill (mPs-~
-F klii)-j-Kna-k ([Leis) sin (m,P8--klii)l;
521ntk i = I - K,-+k ([leis) cos (n3s-I- kpi) --
-i-K,,_,t ([Leis) cos 401.
The functions A 2mki? A 2mki, D2mki, and f22mki are written in the same way, but v is used instead of M.
In deriving Eqs. (5) it was assumed that di and yi were independent of angle. From Eqs. (5) we can find the
criticality condition for the present problem if we restrict ourselves to a k-th order approximation; we obtain a sys-
tem of 2N (2k+ 1) linear homogeneous algebraic equations, the vanishing of whose determinant is the criticality con-
dition for the problem under study. The effectiveness of the rod system will be characterized by the difference Keff
between the cases with and without absorber rods in the reactor. In most of cases encountered in practice we can
restrict ourselves to a zero-order approximation (k= 0), and its is only for large absorber diameters that we must use
one more term of the expansion in k [2]. If the rods are placed at equal intervals along the circumference of a
circle, this solution becomes the solution obtained in [1]. In this case, in Eqs. (5) the constants Ptmi, P2mi should
be taken equal to zero, since the problem becomes symmetric with respect to tP and wi (if the angles are counted
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from the polar axis passing through the center of the reactor and the center of any rod). The functions Ajmki,
A2mki, as well as Etn, E2n, Fin, F2n, Htn, and Hen in Eqs. (1), (2) vanish for the same reason.
The problem is solved in a similar manner for an arbitrary distribution of the system of absorber rods in the
active zone of a reactor with a reflector (lack of space prevents us from stating the solution).
The authors thanks N. N. Ponomarev-Stepnoi for his valuable advice and assistance in developing methods
of calculating the efficiency of control. units in a reactor with a reflector.
1.
V. I. Nosov, Atomnaya 6nergiya, 9, 262 (1960).
2.
V. I. Nosov, Atomnaya dnergiya, 10, 269
(1961).
3.
V. I. Nosov, Atomnaya 6nergiya, 12, 326
(1962).
4.
G. N. Watson, Theory of Bessel Functions [Russian translation], Moscow, Izd-vo inostr. lit. (1949).
740
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FREQUENCY ANALYSIS IN A SYSTEM WHICH INCLUDES A RUNAWAY REACTOR
A.. R. Mirzoyan and I.' N. Brikker
Translated from Atomnaya Energiya, Vol. 15, No. 1,.
pp. 74-76, July, 1963
Original article submitted October 2, 1962
The frequency analysis of feedback systems which include a reactor requires a knowledge of the transfer func-
tion of the kinetic reactor. When the reactor operates at a constant power level, this function is known [1]. How-
ever, the transfer function given in [1] cannot be used for the frequency analysis of runaway reactor operation.
Neutron Period-measuring unit
Lo aritFm Di erentiator
Reactor detector unt T Comparator
Rods nf(p) n I=A ?n I U=x,enI U alit
Fig. 1. Automatic control system for maintaining constant period.
F(4p)
Period
controller
YO if K2
70 Z0
Fig. 2. Functional schematic describing the process of period control.
An attempt was made in [2] to obtain the transfer function for a runaway reactor. Because of the "algebraic"
difficulties, however, it was not obtained in Laplace transform expressions in [2]; only a harmonic analysis of a runa-
way reactor was given.
In the present study we derive such a transfer function in explicit form and give a block diagram for a period
control circuit. This enables us to analyze automatic reactor start-up systems by frequency methods.
Let us consider the case of runaway in a reactor with a period ro. If the runaway proceeds ideally, the steady-
state neutron flux will change exponentially ni(t)= noel/r0 (where no is the initial neutron flux level). The excess
reactivity po corresponding to this process remains constant. However, in controlling the runaway the period r de-
viates from the given value ro. This deviation is caused by the oscillation of the excess reactivity p about po. We
will therefore have, superimposed on the steady-state exponential function, neutron flux oscillations caused by the
control reactivity: Ap(t)= p(t)-po.
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p--
Actuator
Sn (t) = n (t) - n1 (t) 1
n1 (t)
I (1)
it (t) =ni (t) [1+Sn (t)], J
where n(t) is the instantaneous value of the neutron flux. We
shall assume that 6 n(t) is small; that is, 16 n(t) I 25 kG, a broad spread in the results is observed and the dependence on H becomes a weak
dependence.
Measurements of the temperature of ions heated by means of ion cyclotron waves were carried out on the
stellarator B-66, and showed that the peak ion temperature attains 250 eV, declining rapidly after the B4-generator
is switched off (time constant -20 psec). The measurements were carried out by means of a diamagnetic loop and
an ion energy analyzer.
Plasma instability was studied in the Table Top (the Livermore magnetic trap with mirrors). It was shown that
channel instability arises solely within a specific range of plasma density values. When plasma is injected from a
titanium source (W. Perkins) along the axis of the system, and is subsequently compressed by the fast magnetic field
of the mirrors (compression time 80.35 and 16 psec), the fact was noted that the plasma pinch departed from the
axis of the magnetic trap and began to rotate about that axis at an angular velocity w =107 sec-1. The principal
field varied only very slowly (7500 and 460 psec).
In experiments on the interaction of a plasma obtained by means of a coaxial injector (v =106 cm/sec) and
the magnetic field of a magnetic mirror (H= 25 kG), reflection of the deuterium plasma from the mirror was ob-
served (J. Marshall), accompanied by the emission of neutrons at an intensity 5. 106 neutrons/burst.
A. England used the method of electron cyclotron resonance in a resonator placed in a magnetic field of mir-
ror configuration to obtain, under stationary conditions, a plasma of density 1012 particles/cm3 with hot electrons
(Te = 50 keV) and cold ions. The neutron yield from the plasma was 105 neutrons/sec. Most of the neutrons had
energies below 1 MeV.
B. Motley and associates studied, on Q machines, excitation, propagation, and collisionless absorption of ion
acoustic oscillations in alkali plasmas. Ion-acoustic oscillations in the 104 to 105 Hz frequency range were excited
and detected in a strongly ionized plasma of 5.1010 to 5. 1011 density by means of a tungsten grid immersed in the
plasma. The measured phase velocities showed no dispersion, and were 0.7 of the phase velocity predicted by theory
for a collision-free isothermal plasma at Te= 2300?K. The attenuation length was independent of plasma density.
Measurements of the energy of protons leaving a 300-kilovolt plasma because of charge transfer during the
time of plasma buildup were carried out on the DCX-1 machine, simultaneously with other experiments (measure-
ments were carried out both in the stable state and during the decay of the plasma). It was shown that protons have
an energy spectrum with a half-width of 20-60 keV. The fact was established that the half-width depends strongly
on the injection current and on confinement time. The ion energy ranged from 100 to 300 keV. Intense radio-fre-
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quency bursts were observed at 14 Mc frequency, corresponding to ion cyclotron oscillations. The duration of the
bursts was -2 to 3 hundredths of a second, and the time between pulses 0.1 sec. At the initiation of a burst, the slow
electrons move out through the mirrors; the positive potential of the plasma increases. At the end of a burst, the
reverse electron current reduces the potential to the previous value. As the oscillations arise, there is also a related
increase of fast proton losses through charge transfer. The suggestion was advanced that these irregular phenomena
are related to the heating of the cold plasma in an ion cyclotron instability.
Three papers were devoted to plasma phenomena in solids. It was shown that a whole series of purely plasma
effects such as the pinch effect, excitation of waves, etc., may be observed even in semiconductors.
Of special interest among the theoretical papers presented, we here single out contributions by D. Dowson and
K. Smith, who made computer studies. of the development of double-flow instabilities and anomalous resistivity in
a collision-free plasma. They considered a model of a one-dimensional plasma consisting of a large number of
charged infinite planar layers. The "plasma" was neutron on the average (1000 positive and 1000 negative particles
per unit length). The mass of an "ion" was equal to 25 "electron" masses. The velocity distributions of the ions
and electrons were Maxwellian, shifted by AV with respect to each other. This problem simulates the behavior of
a real plasma when a current is passed through the plasma. Theory predicts that, at sufficiently large AV in the
plasma, instability should ensue. However, a theoretical treatment of the nonlinear phase of the process of develop-
ment of this instability would be extremely difficult. Dowson and Smith ran two cases on the computer: AV= 0.6
Vte and AV = 2.5-Vie, where VLe is the mean thermal velocity of the electrons. The value of the current flowing
through the plasma remained fixed. The computations revealed that the velocity distribution of the electrons be-
comes smeared out at AV= 2.5?Vte during a time t -60/cape (wpe being the plasma frequency) with an instability
developing at the point (the mean energy of the electrons is approximately doubled), and that the growth of the os-
cillations comes to a halt later on. During the development of the instability, an anomalous resistivity R is observed
for a current I0, which may be computed as dW /dt = RIp 2 . These results confirm the qualitative ' inferences of the
theory.
After the conference, the members of foreign delegations visited the physics laboratory at Princeton University,
where they were familiarized with all the existing experimental facilities.
STATUS OF THE URANIUM INDUSTRY IN THE CAPITALIST COUNTRIES AS OF 1962
V. D. Andreev
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 88-91, July, 1963
During the years 1960 to 1962, uranium demands reached about 30,000 tons a year, 25 to 30% below the
level prevailing in the years 1959 and 1960. As a result of the drop in demand, the curtailing of uranium ore min-
ing operations and the drop in production of concentrates continued apace, with underutilization of production fa-
cilities a commonplace. According to estimates, 30,800 tons ofU3O8 were produced in 1962, 7% below the 1961 level.
1961 production fell 11% below the 1960 level.
The demand for uranium on the part of the nuclear power industry increased at a far slower rate than that anti-
cipated. The discovery of large deposits of petroleum and gas, and the appreciable stepping up of production of
fossil fuels liquidated the fuel deficit plaguing western Europe, and a sizable drop in specific capital investments
and in the cost of electric power at conventional power stations imposed much more stringent requirements on nu-
clear power stations. (As an example, in order for the construction of nuclear power stations to be a profitable ven-
ture in the USA, the costs of electric power production at nuclear-fueled stations would have to be lowered not to
0.8 cents/kW -h, but the low figures of 0.6 or 0.65 cents/kW -h.) As a result, the power output of nuclear power stations
in the capitalist countries will not exceed 10 million kW in 1967, as against 25 million kW envisaged back in 1957.
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TABLE 1. Industrial Uranium Reserves in the Capitalist Countries
Ore re
serves,
U308 content in ore
Data
millio
tons
ns of
at start
of year
Total
900-920
1963
Union of South Africa
952
.4
0.034
324
1959
Canada
273
.1
0.121.
252.2
1962
USA
60
.7
0.28
170
1963
India
15
.7
0.3
47
1960
Australia
0.1-0.3
25?
1962
France
0.1-0.3
21
1963
Gabon
20
.0
0.5
6.01
1963
Argentina
10.0
1962
Southwest Africa
3
-5.0
0.22
7-10
1962
Spain
2
.0
0.1-0.4
^-4.0
1963
Italy
0
.6
0.12
0.72
$
1962
Japan
3
.0
0.05-0.2
1.5-6
1962
Switzerland
0.02-0.1
2.0
1963
Mexico
1
.05
0.1-0.2
1-2
1963
West Germany
0.
3
0.1-0.2
0.4
1962
* 12.5 thousand tons fror
tOnly in ores containin
$ Data based solely on o
at 14,000 tons U308.
g 0.5% U3O8.
ne deposit; geolo
TABLE 2. Quantity of Fission Energy Contained in Atomic Ore Reserves in the USA, in
1018 Kilocalories [8]?
Energy in U235
Total energy content
Cost, $/kg
Including proved
and probable
reserves
Including proved
and probable
reserves
U3O8
0-22
0.1.
0.04
12.6
5.544
22-26
0.756
0.043
10.08
6.048
66-220t
2.52
1.26
352.8
176.4
220-11001
226.8
55.44
30,240.0
7,560.0
Th02
0-22
-
-
6.3$
1.512$
22-66
-
-
3.28$
1.512$
66-220t
-
-
554.4
176.4
220-11001.
-
-
47,880.0
15,876.0
* Fission energy content computed on basis of assumption that all materials will be ulti-
mately fissionable after being cycled through reactor cores. Losses incurred in recovery
of spent nuclear fuel and other relatively small losses were ignored in the calculations.
tIn winning uranium and thorium from granite, and uranium from bituminous schists
and phosphates.
$ Only incomplete data available.
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TABLE 3. Mining of Uranium Ore in the Capitalist
Countries, Millions of Tons [14-17]
I ' Country
USA
0,25-0,27
3,0
7,2
7,3
Canada
Un. of S. Africat!
6,1-0,10
1),035
G,O
20,0
10,1) *j
21,0
8:(I *t
15,5
12,(I
Australia*
U,2
0,2
France
(j
(1 !)
0,8
0.ti
*
Estimate.
T Processed at mills.
Some countries (India, Mexico, Argentina, the
UAR, and others) are attempting to supply their own
needs in the production of nuclear raw material, albeit
in modest quantities.
Uranium needsin the USA and in Great Britian
are supplied by deliveries meeting terms of contracts
drawn up back in the mid-fifties. France, Sweden, and
Japan are attempting to cover their atomic raw ma-
terials needs primarily by arranging their own domestic
production, since uranium imports entail obligations
which those countries tend to view as burdensome and
unacceptable. All of this contributes to a deterioration
in the position of the world's largest uranium exporters,
Canada and the Union of South Africa.
TABLE 4. Uranium. Production in Capitalist Countries in Tons U308 [1, 3, 18-21]
1962 *
Total
21,700
37,000
33,000
30,800
USA
7,840
16,140
15,785
15,504
Canada
5,950
11,380
8,764
7,665
Union of South
Africa
5,170
5,826
4,971
4,500
Australia
360
1,000
1,350
1,200
Francet
296
984
1,187
1,060
Gabon
321
5 47
Malagasy
Republict
72
80
Portugal$
1,492
450
Spain*
54
55
West Germany*
11
11
Argentina*
18
14
10
Italy**
1
8
Congo
1,500
1,080
* Estimate.
tContent of metallic uranium in concentrates.
$USA imports; weight of uranium concentrates, not content of uranium oxide in concen-
trates. Coarse concentrates containing about 10% U308, to judge by cost figures, are pro-
duced in the country.
** Previous available estimates: 75 tons for 1960 and 130 tons for 1961 refer to planned
production figures. Because of the overproduction and drop in world market prices. Italy
has not arrived at industrial assimilation of its own deposits.
Changes in the raw materials base. The proved industrial reserves of uranium in the capitalist countries (see
Table 1) has shrunk noticeably during the past three years. This is due to the contracted volume of geological pros-
pecting activities for uranium and to the very large-scale mining operations in progress. During these years, over
100 million tons of ore containing from 110 to 115 thousand tons of U3O8 were mined and processed.
About 50 million tons of ore were mined in Canada during the years 1958 to 1962, while no significant new
deposits were discovered, the upshot being that industrial ore reserves ended up 2010 less than in 1957 (the 1957 fig-
ure was computed at 342 million tons) [7].
The industrial reserves of uranium ore in the USA were likewise sharply revised downward, by as much as 25%
over the years 1960 to 1962. According to USAEC estimates, industrial reserves of uranium in the USA will be cut
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down to 90 thousand tons of U308 by 1967. One of the factors behind this scaling down of prospecting and explora-
tion work was the decision by the AEC to purchase ore, up to 1966, solely from deposits which were operational prior
to 1958.
In an official USAEC report presented to the President in November, 1962, the total quantity of fission energy
contained in the nuclear raw materials reserves in the USA were estimated at79,290 billion kilocalories, which is
many times in excess of the fossil fuel resources (Table 2).
Geological propsecting for uranium and exploration of deposits are continuing in western European countries
(France, West Germany, Italy, Austria, Sweden), Asia (Japan, India, Pakistan), in Africa (United Arab Republic,
Kenya, Tanganyika), Latin America (Argentina, Mexico, Peru).
TABLE 5. Uranium Ore Processing Mills
In operation
Under con-
struction or
planned in
1962
Total daily capacity, thousands
of tons of ore
125
120
100
lo capacity in use
88
80
70
Number of concerns involved
84
71
67
9*
USA
25
26
27
3
Union of South Africa
17
13
12
Canada
17
8
8
Australia
5
5
3
France
4
4
4
Gabon
1
1
Malagasy Republic
1
1
Spain
1
1
Portugal
1
1
West Germanyt
1
1
A rgentina$
3
3
Italyt
1
1
Japant
1
1
Indiat
1
1
Swedent
1
Mexico$
1
Brazil$
1
Congo
Finlandt
N. Rhodesia
? Of which two have been complet
tPilot plant.
$ Experimental facility.
ed.
Recent data place the total (geological) reserves of uranium ore in France, Gabon, and the Malagasy Republic
at 60,000 tons U3O8, and proved reserves at 21,000 tons in France proper and 6,000 tons in Gabon (Mounan)[3].
In Sweden, in the Norroker district, bituminous schists with a higher uranium content than those at the Ranstad
deposit were found in 1962, and a processing mill is being built to handle them [9].
Despite the intensified program of prospecting, no large uranium deposits were discovered in West Germany.
The reserves at the Wohlsendorf (Bavaria) deposit were estimated at 100,000 tons with 200 tons U3O8 content. The
mean uranium content in the ore is. comparatively high: 0.216 U3O8; however; the depth at which the ore lies makes
mine operations unprofitable [3]. The Waisenstadt (Bavaria) deposit contains. 60 to 75 tons U3O8. The reserves at the
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deposit in the Elweiler district, the only one presently being worked in West Germany, are estimated at 100 tons
U308 with a mean U308 content in the ore of 0.1% [10]. The uranium reserves contained in the uraniferous anthra-
cites of Upper Bavaria discovered in 1962 are estimated at several hundred tons. It is supposed that new zones of
uranium content higher than that found in presently known deposits may be found in the coal fields of Upper Bavaria [11].
A uranium ore deposit was discovered in 1962 at Schwarzwalf in the Menzenshwand district. The U308 content found
in an assay of 300 tons was very high: 1 to 1.4%. This indicates a vein type deposit whose reserves are probably
modest, however [12].
Mexico's reserves of uranium have seen an appreciable increase. In mid-1962, the figure for total reserves
of uranium ore stood at 0.4 million tons. An estimate at the year's end placed the level at 1.05 million tons [2, 13].
Several uranium deposits were discovered in India during 1962, particularly in the Kangra district in western
Punjab [3].
News was published on the discovery of a promising uranium deposit in Peru in 1960, in the Vilcabamba dis-
trict. However, operations would be unprofitable given the low market prices prevailing and the overproduction
conditions [3].
On the basis of data on the number of mines in operation, their output and the production of concentrates, we
may assume that mining of uranium ore underwent a curtailment during 1962 in the capitalist countries (Table 3).
This curtailment in mining operations extended for the first time to all the major mining countries.
TABLE 6. USAEC Purchase Prices for Uranium Concentrates
Dollars/kg U308 [1, 24]
Suppliers
1959-1960
1960-1961
1961-1962
American
19.78
18.79
18.04
Canadian
24.49
24.00
21.89
Miscellaneous (Union of
South Africa, Congo,
Australia, Porugal)
26.42
25.92
25.26
Average prices
22.42
21.38
20.13
Mining of uranium ore in the USA was reduced 14% below the 1961 level. The U3O8 content in mined ore
was 15.3 thousand tons as against 17,000 tons the previous year, i.e., 10% lower, attesting to the increase in the
mean U308 content in the ore mined.
In 1962, by our estimate, the production of uranium concentrates dropped 2.2 thousand tons of U3O8 as against
1961 (Table 4). The drop in Canada was greater (a 13% drop) as in the Union of South Africa (10%). The USA
accounted for about 50% of the uranium production in the capitalist world during 1962.
Canada and the Union of South Africa, which boast the largest uranium ore reserves in the capitalist world,
are being converted into virtually second-rank producers. This position is due to the fact that the USAEC, as the
biggest consumer of uranium raw material, drastically cut purchases in other countries, thus shifting the center of
gravity of its purchases onto American suppliers.
Production of uranium concentrates was cut first in France, by 11% compared to the 1961 figure. However,
the amount of nuclear raw material at the disposal of the French Atomic Energy Commissariat increased by 27%.
This is due to a marked increase in deliveries from Gabon, by a factor of eight over the 1961 figures.
The production of uranium concentrates in France, Gabon, and the Malagasy Republic will probably level off
at 1960 tons of U308 in the coming years [3, 20].
France, in striving to maintain its leading positions in the nuclear industry of the "Common Market" countries
in the years to come, has begun an intensive development of its own raw materials base recently (a huge gas diffu-
sion plant for production of enriched uranium, with a throughput as high as 1.5 thousand tons uranium metal an-
nually, is now being built at Pierrelat).
1962 saw the curtailment of production hit Australia. The processing mill at Radium Hill and the Port Pirie
plant, as well as a small plant in the northern section of the country, had been closed down. The contract for de-
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livery of ore to the Joint Anglo-American Atomic Fuel Agency of uranium concentrates from the Rum Jungle plant
had already expired. The closing of this plant was due to the liquidation of an entire industrial district based on the
uranium mining operations. The government therefore decided to continue ore processing operations, warehousing
the output.
As many as 22 plants, including 3 pilot plants (in Southern Rhodesia, Finland, and Sweden), closed down in the
capitalist countries during 1960-1962, reducing the total production level by roughly 20% (Table 5).
Only one new plant went into operation during 1962, the Carbon County (Wyoming) operation in the USA,
with a daily capacity of 180 tons of ore (450 tons according to data from another source). Two plants were built.
The first, at Ranstad (Sweden) is to have a capacity of 140 tons U308 and is scheduled to go into operation in 1965
[22], bituminous schists with 350 g/ton U308 content will be processed; construction costs are estimated at $28 mil-
lion. As much as 800 thousand tons of ore will be mined yearly to supply the plant, and this will mean working the
mine for 15 years. The concentrate will have the following composition(in percentages): U3O8-84; PO4-0.014;
Na-7.5; Fe-0.04; Mo-0.001; SO4- C02-1,3 [22]. The second plant, located in India (in the Jaduguda dis-
trict of the state of Bihar) is built for -200 tons U308 annual capacity; it is scheduled to go into operation in 1965
[23]. Plans call for expanding mining operations to 1000 tons daily in 1964, to meet the needs of the plant.
Construction of new plants is being planned in the USA (in the state of South Dakota, using as base operation
of the large lignite field in the Bowman area), as well as several small operations in Japan, Brazil, and Mexico.
However, because of the possibility of acquiring low-priced uranium on the market, it is hardly likely that all of
these plans will be brought to fruition.
Price structure. As a result. of the supply swamping the demand, the drop in ore mining costs and concentrate
production costs, the shift to operation of the most profitable mines and plants, 1962 prices continued to decline
(Table 6).
In 1960, an agreement was signed between Canada and Great Britain for the delivery of 10.9 thousand tons of
U308 to Great Britain over the 1963-1966 period, with the price averaged at 11.07 dollars/kg U3O8.
1. V. D. Andreev, JAE, 13, 293 (1962),
2. Metal Bulletin, No. 4763, 15 (1963).
3. Atomwirtschaft, VII, 618 (1962).
4. New York Times (September 23, 1962).
5. Metal Bulletin, No. 4743, 20 (1962).
6. Mining J., 258, 547 (1962).
7. J. Griffith, Canadian Mining J., 84, 97 (1963).
8. USAEC, Civilian Nuclear Power. A. Report to the President-1962, Washington (November 20, 1962),
9. Mining J., 259, 153 (1962).
10. Gluckauf, 97, 1028 (1961).
11. Industriekurier, p. 557 (Beilage) (September 5, 1962).
12. Atomwirtschaft, VII, 465 (1962).
13. Engng. and Mining J., 163, 180 (1962).
14. V. Andree, JAE, 11, 73 (1961).
15. Mineral Trade Notes, 55, 70-71 (1962).
16. American Metal Market (February 7, 1963).
17. Commissariat a 1'energie atomique. Rapport Annuel, 1960,, Paris (1961).
18. D. Baker and E. Tucker, Minerals Yearbook, 1961, Washington (1962).
19. Statistical Summary of the Mineral Industry, London (1962).
20. R. Bernick, Engng. and Mining J., 164, 117 (1963).
21. Northern Miner. (January 3, 1963),
22. Nuclear Power, 8, 54 (1963).
23. India News (May 4, 1962).
24. Appl. Atomics, No. 371, 7 (1962).
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USAEC D'ELEGATION`VIS`ITS -THE SOVIET UNION '
A. A.
Translated from Atomnaya Energiya Vol.-1 5; No. 1,
pp. 91-93, July, 1963
In response to the an'invitation tendered by the chairman of the State Committee on the Uses of Atomic En-
ergy of the USSR, a delegation of the US Atomic Energy Commission headed by AEC chairman Glenn T: Seaborg,
made an official visit to the Soviet Union from May.19 to May 30 this year (1963). The delegation included the .
chairman' of the AEC consultative' committee, Manson Benedict, the' AEC general manager A. Luedecke, the head
of the international affairs board A. Wells, the director of the Argonne'National-Laboratory, A. Crewe, the president
of the Association of-Midwestern Universities,- G. Tape, staff member A.'Ghiorso of the Lawrence: Radiation Labora-
tory, staff member A. Zucker of the Oak Ridge National Laboratory,.and'technical adviser to the AEC chainman
A. Fritsch, assistant to the AEC chairman, C,. King.
A?. M. Petros' yants . and Glenn T. Seaborg (left) after?"signing the Memorandum.
On the day following their arrival, the American delegates were welcomed by the chairman.of theUSSRState-
Committee on the Uses of Atomic Energy', A. M. Petros'yants. During their introductory chat, they discussed the
agenda.of the official visit and the text of a joint memorandum on; collaboration in the field of the peaceful'uses
of atomic energy. On the same day, the American scientists visited Moscow State University, the Physics Institute
of the USSR Academy of Sciences, and the Institute 'of Chemical Physics of the USSR Academy of Sciences. At Mos-
cow State University; 'the -guests inspected the auditory, the-students dormitory quarters, and several :laboratories, in-
cluding the cosmic radiation laboratory.
On May 21, the delegation met with the president of the USSR Academy of Sciences, M. V. Keldysh.
At the Institute of Atomic Energy, which was visited on May 22, the guests were shown the linear electron ac-.
celerator, the cyclotron, the reactors, and several laboratories. Of the many thermonuclear machines there, the PR-5
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facility, an adiabatic trap with combined magnetic field, with which Soviet physicists have recently achieved an
enormous success by confining a plasma in the stable state for 10-15msec, was demonstrated. At the Institute, Dr.
G. Seaborg delivered a lecture on the transuranium elements to the Soviet specialists present, and was heard with
rapt interest.
On the following day, the American specialists traveled to Obninsk, to see the Physics and Power Engineering
Institute there. There they were shown the World's First Nuclear Power Station, the BR-1 and BR-5 fast reactors, a
portable nuclear power facility, and the sodium laboratory.
During their visit to the Nuclear Reactor Research Institute situated near Ul' yanovsk, the attention of the dele-
gation was drawn to the operating reactor CM-2, the miniaturized nuclear organic-cooled power assembly, and a
boiling-water reactor now under construction. The members of the American delegation voiced high praises for the
CM-2 reactor.
On the next two days, the American scientists spent their time in Leningrad At that point they were for the
first time divided up into two teams: one headed up by G. Seaborg visited several laboratories of the Radium In-
stitute, while the other team was received by specialists of the Physics and Engineering Institute of the USSR Acad-
emy of Sciences. In the evening, the entire delegation visited the Electrophysics Equipment Research Institute, where
they were familiarized with the activities of the Institute, with its laboratories, and where they were shown a number
of operating and partially completed thermonuclear and accelerator facilities, including the "Al'fa" toroidal ther-
monuclear machine, and a linear accelerator designed for medical research.
The members of the American delegation also stayed at the Physics and Engineering Institute in Kharkov,
where they saw demonstrations of the linear accelerator for multiply-charged ions and the large 2 BeV linear elec-
tron accelerator.
On May 28, the delegation visited the Joint Institute for Nuclear Research at Dubna. Here the American spe-
cialists were informed on the latest work of the Nuclear Reactions Laboratory, where, as is generally known, a group
of Soviet scientists recently scored a great success in synthesizing the new element 102, of mass number 256, on the
multiply-charged ion cyclotron. The guests also inspected the pulsed fast reactor at the Dubna Institute.
On May 27 and 29, the American delegation paid visits to the construction site of the Novo-Voronezh nuclear
power station and to the Serpukhovo 70 BeV proton accelerator.
On May 29, G. Seaborg was received in the Kremlin by the Chairman of the Presidium of the Supreme Soviet
of the USSR, L. I. Brezhnev. A. M. Petros'yants took part in the discussion.
In the course of the visit, talks were conducted between the State Committee on the Peaceful Uses of Atomic
Energy of the USSR and the US Atomic Energy Commission, concluding on May 21 with the signing of a Memoran-
dum on collaboration in the field of the peaceful uses of atomic energy.
The Memorandum establishes an extensive program of scientific and technical exchanges with the purpose
of developing and further expanding collaboration between the USSR and the USA in the field of the peaceful uses
of atomic energy.
An understanding was arrived at on mutual visits of teams of specialists to promote the familiarization of col-
leagues of both countries with the status of scientific research in the following areas: nuclear power reactors includ-
ing fast reactors and superheat reactors; plasma physics and controlled fusion; nuclear physics and the physics of high-
energy particles; solid state physics; decontamination and burial of radioactive wastes; applications of labeled com-
pounds in medicine, radioneurological research; design and operation of accelerators. The dates of the visits, their
duration, and the composition of the delegates will be subject to further agreement in each specific case.
The Memorandum also provides for protracted transfers (for periods up to one year) of specialists on controlled
thermonuclear fusion, reactor engineering, and high-energy particle physics in research laboratories, for the purpose
of sharing practical experience and studying the operation of existing facilities and equipment.
Exchange of scientific information (books, papers, preprints) will be promoted, with lectures scheduled in those
fields of scientific activity where exchanges of delegations occur. The Memorandum sets the amount of information
to be exchanged and the information exchange periods. The Memorandum also provides for the simultaneous trans-
mission of information intended for bilateral exchange through the International Atomic Energy Agency.
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Two joint scientific conferences were decided upon. A conference will be held in the USSR on low-energy
nuclear physics, and another in the USA on the decontamination, solidification, and burial of radioactive wastes.
Agreement was reached on exchange of scientific instruments. The conditions governing this exchange will
be discussed further within the framework of the laws and export practices of the two countries.
The Memorandum envisages the possibility of taking supplementary measures to promote collaboration be-
tween the two countries and sets the dates for taking action and the procedure for extending the terms.
The text of the Memorandum was signed by the State Committee on the Uses of Atomic Energy of the USSR,
represented by A. M. Petros'yants, and by the US Atomic Energy Commission, represented by Glenn T. Seaborg.
In summarizing the significance, effects, and benefits of their visit to the USSR, Glenn Seaborg and the mem-
bers of the American delegation stated, at a press conference on May 30, that the delegation received a warm wel-
come. Our guests, Seaborg stated, were most hospitable and did everything possible to render our visit useful and
profitable; we saw everything we set out to see. The view of the American scientists is that the Soviet Union has
made tremendous strides in many areas of the peaceful uses of atomic energy. In these remarks, they of course in-
clude, for example, thermonuclear research, reactor design, and the study and production of transuranium elements,
as well as other subjects.
771
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Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 93-95, July, 1963
USSR. A coincidence scintillation spectrometer has been built at the Latvian nuclear reactor. This instrument
is capable of recording several tens of thousands of gamma pulses resulting from neutrons bombarding atomic nuclei,
in a fraction of a second. Physicists of Latvia and the other Baltic republics will be greatly aided by this new fa-
cility in their study of rare earths at the reactor.
USSR. Patent No. 146414 has been issued for a technique of producing sample radioactive gaseous sources with
the special feature that a low-boiling radioactive liquid, the quantity and activity of which are already measured by
conventional absolute techniques, is vaporized into a known sealed volume, in order to facilitate a wider use of rela-
tive methods of activity measurements.
The specific activity (a) of the organic liquid labeled with a beta-active isotope is carefully determined when
the proposed method is used. Several milligrams of this liquid are then collected in a tiny glass bead ampule crimped
on the end, the ampule is sealed, and the amount (m) of the material taken is determined before and after sampling
by the difference in weight. The activity (A) of the sample is determined from the relationship A = a ? m. The am-
pule is then placed in a suitable pressure-tight chamber and crushed inside. At this point the volume of the cham-
ber must be sufficient to allow for complete evaporation of the radioactive liquid. After the sample of radioactive
liquid has been evaporated, a gaseous radiation source results, with the activity precisely known and, once the vol-
ume of the chamber is known, we will have no trouble computing the activity contained in any part of the chamber.
USSR. A new method for separating potato tubers from stones and clumps of ground during harvesting opera-
tions involving the use of special machines has been developed at the All-Union Institute of Agricultural Mechan-
ization. This method is based on the contrasting penetrability of gamma rays through potato tubers and through
foreign matter. The potato tubers are sorted out on a turntable at the edge of which is positioned a circular con-
veyor with movable lift fingers. When the potato tubers come into the area being monitored, absorption of gamma
radiation is minimal. But as soon as lumps of dirt or stones make their appearance, absorption rises steeply. Relays
instantly feed a command to a reject mechanism, which proceeds to eject the foreign matter without delay into a
special hopper.
USSR. A seminar was conducted at the Kadamjai mine (in Kirghizia) on applications of radioisotopes in min-
ing. The seminar made a special point of the successful use of logging instruments incorporating gamma sources, in
delineating the boundaries of rock and ore bodies, and in locating metal in rocks and assaying the metal percentage
content in ore.
USSR. A seminar was conducted at Aktyubinsk at the chromium compounds plant, dealing with experience
on the incorporation of radioisotope and nuclear radiation know-how into production. The seminar took specialnote
of the use of instruments using radioactive sources in many process control applications.
USSR. Radioisotope instruments are currently in widespread use in the Donets region. Over 300 such instru-
ments were in regular use at the beginning of 1963.
USSR. A radiological division was inaugurated at the P. Stradyniua clinical hospital in Riga (Latvia). Patients
are accommodated in two-bed wards with specially designed shielding walls. During active cobalt therapy, contact
with the medical staff is maintained by telephone; a closed-circuit television hook-up is being installed. The new
radiological division boasts the latest in Soviet-manufactured gamma-therapeutic facilities.
USSR. An "Atoms for Peace" exhibit on wheels organized by the USSR State Committee on the Uses of Atomic
Energy and the local Polytechnic Museum has been open to the public for some time in Vladivostok. In addition to
the usual stands, the exhibit is demonstrating a sizable number of operational instruments and working mock-ups.
A seminar was conducted during the exhibit for the benefit of laboratory staff members and workers in industrial
establishments in the area.
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IAEA. In April, a conference of experts on methods of assessing cost factors in nuclear power stations coupled
into national power grids, and surveying the effect of nuclear power station operations on the performance and cost
picture of conventional power stations coupled into the national power grid was held in Vienna. Eleven experts from
11 countries (Brazil, Great Britain, Hungary, India, Italy, USSR, USA, France, West Germany, Sweden, Japan) par-
ticipated in the conference, along with 10 observers including two from Euratom and one from the UN European
Economic Commission.
The conference placed the following points on its agenda: 1. differences between nuclear-fueled and fossil-fueled power stations operating in the same or different
power systems (service life of station equipment, ability to respond to load and system variations, station off-duty
time, cost structure of electric power at conventional and at nuclear power stations, effect of cost of fuel on the po-
sition of the power stations on the power system load diagram);
2. methods for comparing electric power costs at conventional and at nuclear power stations feeding power
3. comparison of ultimate effects of hooking up a series of nuclear or conventional electric power stations
into the power grid and changes wrought in the performance and cost picture of power stations already forming part
of the grid;
4. cost evaluation of the role played by nuclear and conventional power stations in the power development
programs of underdeveloped countries.
On the basis of the discussions conducted by these experts, and the materials presented by other experts to the
IAEA secretariat, that body is commissioned to prepare a draft document on the economics of including nuclear elec-
tric power stations in national power utility systems, and this report will ultimately by published as an IAEA tech-
nical report.
IAEA. The International Atomic Energy Agency has decided to render assistance to member states in the field
of outer space research, by organizing the collection and rapid delivery of newly fallen meteorites to laboraties for
studies of their radioactivity. The General Director of IAEA has directed a request to all governments affiliated to
IAEA to present a list of interested laboratories and to collaborate in the organization of delivery of new meteorites
to the central organizations of the IAEA in Vienna, thus expediting a rapid distribution of meteoritic specimens to
various laboratories.
East Germany. A research reactor with an Argonaut type annular core went critical at the Rossendorf Central
Nuclear Physics Institute. The 10 kW-rated reactor was designed and built by scientists of the German Democratic
Republic. Nuclear fuel is delivered by the Soviet Union.
Experience accumulated in five years of operating the German Democratic Republic's first research reactor,
2000 kW, was put to use in the design and construction of this pile. The function of the first reactor will now center
primarily on isotope production, studies of solid state physics problems, and neutron physics research.
Poland. At the (Warsaw) State Institute of Hydrology and Meteorology, an isotopes applications laboratory
has been commissioned.
The schedule of operations of the laboratory for the period ahead includes development of methods for spotting
leaks in pipes and ducts (including water pipes) by means of sealed radiation sources, and investigation of ground
water movement by tritium devices. Investigations of tritium content in natural waters, closely related to the above
projects, are designed to establish the rate of turnover of deep-lying ground waters, and this. will aid in determining
the exploitable reserves of underground reservoirs.
Future projects include research on the rate of silt accumulation in riverbeds, harbor bottoms, water basins,
dams and levees, and irrigation systems, and on the mechanisms responsible for silting.
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FROM THE EDITOR
In September 1961 the Committee on Standards, Measures, and Measuring Devices of the Council of Ministers
of the USSR ratified GOST 9867-61, "International System of Units"; therefore, as of January 1, 1963 this is to be the
preferred system of units in all branches of science, technology, and national economy, as well as in teaching.
Bearing in mind the importance of proper preparation for the introduction of the International System of Units
into the national economy and for the proper explanation of the question of units in the scientific and technical
literature, the editor presents in this issue a paper prepared and approved by the Committee on Standards, Measures,
and Measuring Devices of the Council of Ministers of the USSR entitled, "The Introduction of an International System
of Units in the USSR.*
Approved by the Committee on Standards, Measures, and
Measuring Devices of the Council of Ministers of the USSR
THE INTRODUCTION OF AN INTERNATIONAL
SYSTEM OF UNITS IN THE USSR
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 96-98, July, 1963
The development of science and technology in recent years has raised the question of establishing more rigid
requirements for the achievement of more uniform and precise measurements. These requirements have acquired in-
creasing importance as the result of the widespread application of automation and computer controlled technology.
In the latter the units used are among the most important elements of information and therefore the question of
unification of the systems of units is of paramount importance.
In order to satisfy these requirements a rational system of units must be used to measure physical quantities.
In the USSR the following preferred systems of units have been approved as the government standards:
MKS system for the measurement of mechanical and acoustical quantities (GOST 7664-61 and GOST 8849-58)
with the basic units meter, kilogram, and second, and 22 derived units (16 for mechanical and six for acoustical
measurements);
MKSA system for the measurement of electric and magnetic quantities (GOST 8033-56) with the basic units
meter, kilogram, second, and ampere, and 17 derived units;
MKSD system for the measurement of thermal quantities (GOST 8550-61) with the basic units meter, kilogram,
second, and degree Kelvin,* and 12 derived units;
MSC system for the measurement of light quantities (GOST 7932-56) with the basic units meter, second, and
candle, and seven derived units.
Thus, as a whole, the indicated systems involve six basic units, which may be reproduced with the aid of govern-
mental standards using the accepted principles for the determination of these units, and 58 derived units for the meas-
urement of various physical quantities; the latter may be considered composite parts of a unified system of units.
In addition to the indicated systems, the existing government standards for the units of measurement also per-
mit the use of the following systems.
CGS system for the measurement of mechanical, acoustical, electric, and magnetic quantities (GOST 7664-61,
GOST 8849-58, and GOST 8033-56) with the basic units centimeter, gram, and second, and the associated derived
units;
*Provision is made for the use of two temperature scales: the thermodynamic temperature scale and the International
practical temperature scale. The temperatures in each of these scales may be expressed in two ways - in degrees
Kelvin or in degrees Celsius (centigrade).
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MKGFS for the measurement of mechanical quantitites (GOST 7664-61) with the basic units meter, kilogram-
force, and second, and the associated derived units;
The use of the CGS, MKGFS, and mixed units is permitted because they are widely used in practice; however,
it is recommended that the units of the MKS, MKSA, MKSD, and MSC systems be used.
The existence of many systems of units for the measurement of various physical quantities and also of a large
number of widely used mixed units results in significant difficulties and inconveniences associated with the conver-
sion of the numerical magnitudes of the measured quantities from one system of units to the other.
The pressing necessity arose for the establishment of a single, universal system of units to be used in all
branches of science, technology, and national economy encompassing the measurement of mechanical, thermal,
electric, magnetic, acoustic, and light magnitudes.
The most rational system of units to be used in the measurement of the various physical magnitudes is a sys -
tem of units based on six basic units: the meter, kilogram, second, ampere, degree Kelvin, candle.
The preferred system of units in the USSR (six basic, 58 derived) contains all the necessary elements required
for the formation of a single, universal system of units to be used for the measurement of the various physical quan-
tities.
As the result of a detailed examination by and through the agreement of several international organizations,
the International Metrological Organization, the International Standardization Organization (ISO), the International
Union of Pure and Applied Physics (IUPAP), the International Commission on Electrical Engineering (ICEE), etc.,
the question of the unification of the systems of units was solved by the adoption of a single, universal international
system of units based upon the six above-indicated units.
In October 1960 the Eleventh General Conference on Weights and Measures, held in Paris, adopted the Inter-
national System of Units (SI) consisting of six basic units (meter, kilogram, second, ampere, degree Kelvin, candle),
two additional units (radian, steradian), and the 27 most important derived units: this does not prevent the use of
other derived units, which may be added later. All of the six indicated basic units, both supplementary units, and
all of the 27 most important derived units coincide completely with the corresponding basic, supplementary, and
derived units of the USSR government standards using the MKS, MKSA, MKSD, and MSC systems.
On September 18, 1961,GOST 9867-61, "International System of Units,"* was ratified in the Soviet Union and
put into effect as of January 1, 1963. It establishes the preferred use of this system of units in all branches of science,
technology, national economy, and education. This standard does not provide for introduction of a preferential sys-
tem of units for use in the USSR.
The basic merits of the SI consist of the following:
1. The unification of the units used in the various types of measurements.
The SI permits us to use a single common unit of measurement for each physical quantity encountered in the
various branches of technology, e.g., the joule for all types of work and for the quantity of heat rather than the various
units being used at present for this quantity (kilogram-force-meter, erg, calorie, watt-hour, etc.).
2. The system is universal.
The units of the SI cover all branches of science, technology, and national economy, they exclude the neces-
sity of applying other units, and they represent, on the whole, a unified system common to all branches of measure-
ment.
3. System coherence.
In all physical equations using derived units the coefficient of proportionality is always a dimensionless quan-
tity equal to 1.
*Reference to the system of units adopted at the Eleventh General Conference on Weights and Measures is indicated
by the abbreviated designation for the system using the Latin letters SI (the first letters of the words Systeme Inter-
national).
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For example, in the equation for power
N = k(A /t),
where N is the power, A the work, and t the time, if we use the SI, in which the joule is the unit of work and the
second is the unit of time, the unit of power is
1 watt = 1 joule/i second,
where k, the coefficient of proportionality, is a dimensionless number equal to 1.
The use of the Si units significantly simplifies the operations involved in solving equations, in calculations,
and in the construction of graphs and nomograms since the necessity of using a significant number of conversion co-
efficients is eliminated.
4. The structure and interconnection of the SI significantly simplifies the study of the physical laws and the
pedagogical process during the study of general and special scientific disciplines and also simplifies the derivation of
the various formulas.
5. The principles involved in the design of the SI permit the development of new derived units as needed, and
therefore the list of units of the system is open to further development.
Most of the units of the SI have already received wide practical application in the USSR (except for four or five
of the 58 derived units included in the MKS, MKSA, MKSD, and MSC systems).
Let us consider the confusion existing at present regarding the term "weight," which customarily, and as far as
the layman is concerned, is used to denote the characteristic mass (quantity of a substance) even though in mechan-
ics it is used to denote the force of gravity. It is entirely obvious that measures must be taken to eliminate this con-
fusion.
As we know, the weight W is equal to the product of the mass (m) by the acceleration of free fall (s). -
Since the numerical value of Y. varies at different points on the earth the weight also varies, while the mass is
independent of the location at which it is measured. In addition, the term "weight" is often used incorrectly for the
characteristic mass.
In the SI the kilogram is the unit of mass while the unit of force (also the unit of weight) is the newton.
In all cases where we speak of a quantity of a substance, for example, when we speak of the amount of a metal
or of other materials to be used in the manufacture of an article (machine tool, laboratory device, etc.), the mass
must be given in kilograms (or grams, or integral or fractional parts of a gram).
In those cases where it is necessary to determine the lifting force or the weight-lifting force of a tap (fluid) or
the load upon a foundation, etc., we must speak of the weight and express the weight in units of force, i.e., newtons
(or integral or fractional parts of a newton).
The introduction into practical use of the newton as the unit of force rather than the kilogram-force, which is
widely used at the present time, will facilitate the elimination of the indicated confusion and permit us to realize the
advantages achieved as the result of the sharp differentiation between the units of mass (kilogram) and force (newton).
The introduction on January 1, 1963, of GOST 9867-61 does not mean that the use of all of the units of the CGS
system, MKGFS system, and mixed units must cease immediately and that these units must be replaced by units of
the SI in all branches of the nation's national economy.
The introduction into practical. use of units of the SI which have not as yet received widespread use in the na-
tional economy must occur gradually over a number of years, which will vary for each unit, bearing in mind the re-
gion of application of the unit, the instruments used, economic considerations, and other factors. The introduction
into practical use of the SI units should not involve special expenses and should enable us to continue using the exist-
ing measuring devices until the time that they normally wear out.
A small amount of difficulty will be experienced in the introduction into the domestic economy of those units
of the SI which have so far not been widely used in engineering calculations and for the measurement of which we do
not at the present time have adequate instruments, graduated in the corresponding units, e.g., the measurement of
force in newtons, the measurement of pressure in newtons/m2, the measurement of electrical energy in joules, etc.
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Therefore special attention should be paid to the question of transition to SI units for the measurement of force (new-
tons) and pressure (newtons/m2), bearing in mind the presence in the country of an enormous number of machines and
devices for the measurement of these quantities in units of kilogram-force and kilogram-force/cm2, respectively,
and also other units which are widely used at present (kg-force/mm2, etc.).
In a number of cases it is necessary to recalculate in order to convert from the units in current use to units of
the SI. Thus, for example, in order to convert from kilogram-force to newton, we must use the established relation-
ship between the kilogram-force and the newton, namely 1 kgf = 9.80665 n. However, in the overwhelming majority
of cases the conversion may be significantly simplified since within an accuracy of 2% we can assume that 1 kgf = 10 n
and we may use this simple conversion in all cases where it is possible to neglect the 2% difference.
Generally speaking, the accuracy of the allowed rounding off used in the various unit conversions for units of
the CGS and MKGFS systems and mixed units to units of the SI must be separately established for each particular case
taking into account the conditions of application of the given unit.
The entire complex of SI units will be introduced into the scientific, technical, and educational literature (mono-
graphs, questionaries, textbooks, etc.) this year and over the next few years (together with the previously used units).
The introduction of SI units will also affect all norms and other documentation, such as standards, normals, various ob-
jects, technical conditions, etc. Following the order of the Minister of Higher and Intermediate Special Education of
the USSR and the Minister of Education of the RSFSR, the SI will be introduced in all educational institutions.
As a result of the introduction into the national economy of units of the SI which have not as yet received wide-
spread practical application and also of the provision in the domestic economy of measures and measuring devices
assuring the possibility of making measurements in the units of the SI, units not in the SI will not be used in practical
applications (will disappear from the domestic economy). The practical introduction of the units of the SI into the
national economy will be assured by the issue of corresponding tables for converting the measuring units being used at
present into SI units. The conversion tables will include the permissible degree of rounding off. Published question-
aries and textbooks will include methods for converting from one system of units. to the other as required for the vari-
ous physical laws and more expedient methods for replacing the various units now in use with SI units which will be
better suited to the various types of measurements.
The units of measurements used in all standards documents must be indicated. For example, if the SI is in-
troduced in making measurements on an object for which measurements were heretofore made in other units, it is
necessary to preserve the measurements that were taken in terms of the previously used units. We should also proceed
in a similar manner in all cases in which SI units are introduced for technical documentation and means are not avail-
able for making the original measurements in SI units.
. One of the important steps taken is the introduction of SI units not used heretofore in practical applications as
governmental standards for industrial items, raw materials, and general technical and other standards. This step will
be put into effect starting this year. The units of the SI will be introduced in the standards along with the units in
use heretofore in the national economy (that is, the units of other systems or mixed units).
A basic factor in the success of the transition to SI units will be the existence of measures and measuring devices
for all types of measurements in SI units; this is associated with the provision of new scales for measuring devices.
In order to assure the practical use of SI units which have not as yet received wide application it is necessary
to expand and improve the popularization of the advantages of the SI, ensure the publication of the necessary ques-
tionaries and textbooks, reeducate the personnel, and put into effect a series of other measures. Seminars devoted
to the SI would be one way of providing information regarding the SI and of answering questions regarding the prac-
tical introduction of the units. The seminars must be conducted by the more qualified specialists.
Bearing in mind the fact that the publication of scientific and technical literature must precede by a certain
period the direct introduction of the usage of the ST into the national economic practice, the Committee on Standards,
Measures, and Measuring Devices of the Council of Ministers of the USSR directs the attention of the publishers of
scientific and technical books to the necessity of notifying the authors and editors that SI units should be used in
scientific and technical literature that is about to be published in order to ensure the transition to the new system of
units.
In those cases where the newly introduced units of the SI have not as yet received wide application (the new -
ton, newton/m2, etc.) and also in the absence of measuring devices that could be used to make measurements in SI
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units, the new units should be shown together with the units formerly used. The publication of technical literature
and standards documentation and of completed works should not be delayed or re-edited in order to introduce the new
units.
The introduction into national economic practice of all the units of the SI permits us to benefit from the full
advantages of the use of this system in our country, and its international use will facilitate and improve conditions for
scientific, technical, and trade and cultural relations between nations.
A necessary condition.for the successful completion of the work involved in the introduction into the national
economic practice of SI units is active participation in this work and a responsible attitude on the part of large cir-
cles of engineering and technical workers and their searching in each individual case for the most expedient technico-
economic solution.
Acting Director of the Committee on Standards, Measures,
and Measuring Devices of the Council of Ministers of the
USSR
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BIBLIOGRAPHY
Translated from Atomnaya Energiya, Vol. 15, No. 1,
p. 99, July, 1963
D. J. Rose and M. Clark. Fizika plazmy i upravlyaemya termoyadernye reaktsii [Plasma physics and controlled fis-
sion]. Translated from the English, Plasmas and Controlled Fusion, MIT Press, 1961. 1963, 480 pp., 2 rubles,
37 kopeks.
This item is written as a textbook for seniors and graduate physics students interested in plasma physics and
controlled thermonuclear reactions.
The first twelve chapters of the book present the fundamentals of plasma physics, magnetohydrodynamics, the
elements of gaseous electronics in combination with the theory of transport processes and electrodynamics. The next
four chapters elucidate the basic principles and present status of research in the controlled fusion field, and outline
the problems involved in extracting energy from hypothetical fusion reactors.
The appendices provide: a glossary of notations used in the book, interrelation of various systems of units,
frequently used vector relationships, and frequently encountered physical constants.
Stroenie i svoistva splavov urana, toriya i tsirkoniya [Structure and properties of uranium, thorium, and zirconium
alloys]. Symposium edited by 0. S. Ivanov, 1963, 380 pages, 1 ruble, 34 kopeks.
Forty articles appear in this symposium. They detail the results of experimental studies on the structure and
properties of uranium-, thorium-, and zirconium-base alloys, and on the structure and transformations of several
other systems; phase diagrams of binary and ternary systems, and phase transformations are discussed; ample data
are provided on the mechanical and corrosion resistance properties, strength, and creep behavior of alloys contain-
ing uranium, thorium, and zirconium.
A. I. Bezgubov, Yu. I. Byvshikh, P. K. Dement'ev, Ya. M. Kislyakov, L. V. Kovalev, V. N. Kotlyar, V. G. Kruglova,
L. S. Rudnitskaya, and V. M. Tsyrul'nikov. Uran v drevnikh konglomeratakh [Uranium in ancient conglomer-
ates]. 1963, 188 pages, 95 kopeks.
This book draws inferences from available data on foreign uranium deposits associated with ancient conglom-
erates, and points out the governing laws of formation of mineralization as an aid in spotting signs of ore. The first
part of the book deals with the Witwatersrand uraniferous and auriferous district, and the second part with the Blind
River reserves which are in no way inferior to the Witwatersrand. The third portion of the book presents information
on the Jacobina ore district in Brazil, while the fourth deals with uranium manifestations in ancient conglomerates
of Gabon, Chana, and some other countries The fifth and last part presents an analysis of extant hypotheses on the
genesis of ancient metalliferous conglomerates.
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ARTICLES FROM THE PERIODICAL LITERATURE
Translated from Atomnaya Energiya, Vol. 15, No. 1,
pp. 99-104, July, 1963
I. Nuclear Physics
(Nuclear reactions, neutrons, fission of nuclei)
J. Appl. Phys., 34, No. 1 (1963)
0. Oen, et al., 302-312, Ranges of high-energy atoms in solids.
J. Inorg. and Nucl. Chem., 24 (December, 1962)
M. Ramaniah and A. Wahl, 1185-89, Fission of Th232 by 9.5 MeV deuterons. The yield/mass curve.
Nucl. Sci. and Engng., 15, No. 2 (1963)
B. Palowitch and F. Franta, 146-57, Measurement of the temperature coefficient of resonance absorption in
uranium metal and uranium oxide.
I. Asplund-Nilsson, et al., 213-16, Mean number of fast neutrons emitted in spontaneous fission of Um and
Pu
Nucleonics, 21, No. 4 (1963)
J. Waters, 74-76, Measuring particle velocities with Cherenkov rings.
Nuvo Cimento, 27, No. 2 (1963)
H. De Carvalho, et al., 468-74, Fission of uranium, thorium, and bismuth by 20 BeV protons.
II. Plasma Physics
Doklady Akad. Nauk SSSR, 147, No. 5 (1962)
Yu. L. Klimontovich, 1063-66, Note on the statistical theory of homogeneous isotropic turbulence in a rela-
tivistic plasma.
L. S. Solov'ev, 1071-74, On the Stability of a cylindrical plasma jet in a magnetic field.
Zhur. tekhn. fiz., 33, No. 3 (1963)
V. E. Golant, 257-62, Effect of collisions between like charged particles on plasma diffusion across a strong
field.
A. V. Gurevich and Yu. N. Zhivlyuk, 276-90, On the heating of multiply-charged impurity ions in a plasma.
A. B. Berezin, et al., 291-95, Spectroscopic studies on collective motions of N IV ions in the"A1'fa" machine.
V. B. Gil'denberg and I. G. Kondrat'ev, 301-306, Resonance interaction between an electromagnetic field
and higher-order multipole moments of a plasmoid.
V. I. Kogan, 371-73, Gas filter cuts off radiation from particles.
Ahur. eksptl. i teoret. fiz., 44, No. 2 (1963)
L. E. Gurevich, 548-55, Thermomagnetic waves and excitation of the magnetic field in a nonequilibrium
plasma.
A. A. Galeev and V. I. Karpman, 592-602, Tub turbulence theory of a weakly nonequilibrium rarefied plasma
and shock wave structure.
V. D. Shapiro, 613-25, Contribution to the nonlinear theory of interaction between "monoenergetic" beams
and a plasma.
Zhur. ekspt. i teoret. fiz., 44, 3 (1963)
Yu. M. Aleskovskii, 840-45, Investigation of bulk recombination in a cesium plasma.
A. A. Galeev, et al., 903-11, "Universal" instability of a nonuniform plasma in a magnetic field.
Declassified and Approved For Release 2013/02/25: CIA-RDP1O-02196ROO0600110001-6
Declassified and Approved For Release 2013/02/25: CIA-RDP10-02196R000600110001-6
A. B. Mikhailovskii and L. I. Rudakov, 912-18, Note on the stability of.a spatially inhomogeneous plasma
immersed in a magnetic field.
A. B. Mikhailobskii and A. V..Timofeev, 919-21, Cyclotron instability of an inhomogeneous plasma.
Izvestiya vyssh. ucheb. zaved. Radiofizika, 5, No. 6 (1962)
F. V. Bunkin, 1062-71, Emission of a nonequilibrium plasma.
V. N. Tsytovich, 1078-92, Passage of fast particles through a magnetoactive plasma.
L. S. Bogdankevich, et al., 1093-1103, Electromagnetic field noise in a nonequilibriumn plasma.
Yu. A. Kirochkin, 1104-14, Contribution to the theory of noise in magnetohydrodynamics.
Nuovo Cimento, 27, No. 5 (1963)
M. Feix, 1130-37, Propagation of a double-stream instability in a plasma.
Phys. Fluids, 5, No. 11 (1962)
W. Bostick, 1406-1409, Measurement of properties of plasma eddies formed by velocity shear in a magnetic
C. Pan, 1410-15, Some general characteristics of, a two-dimensional incompressible magnetohydrodynamic
R. Levy, 1416-23, Exact solutions to a class of linearized problems of magnetohydrodynamic flow.
J. Menkes, 1414-27, Stability of a heterogeneous shear layer in a magnetic field.
J. Radlow and W. Ericson, 1428-34, Transverser MHD flow past a semiinfinite plane.
N. Krall and M. Rosenbluth, 1435-46, Drift instabilities in a slightly inhomogeneous plasma.
C. Morawetz, 1447-50, Modifications of the structure of a collisionless magnetohydrodynamic wave.
T. Wilson, 1451-55, Structure of collisionless MHD waves.
1. Bohachevsky, 1456-67, Simple waves and shock waves in magnetohydrodynamics.
M. Surdin, 1479-80, Propagation of ultrasonic waves in plasmas.
J. Morris, 1480-81, Damping of quantized longitudinal electron oscillations in a nondegenerate plasma.
K. Halbach, et al., 1482-83, Generation of a hot rotating plasma.
K. Thom and J. Norwood, 1484-85, A new method for measuring electrical conductivity with a magnetic
probe.
Plasma Phys., 4, No. 6 (1962)
N. Allen, et al., 375-90, Toroidal discharge in the Spectrum IV.
T. Fowler, 391-94, Integration of Vlasov equation.
G. Landauer, 395-400, Generation of harmonics of the electron cyclotron frequency in a Penning discharge.
J. Taylor, 401-408, Rotation and instability of a plasma in experiments using fast compression of the fieldBz.
S. Edwards and J. Sanderson, 409-414, A new approach to transport problems in a fully ionized plasma II.
H. Teh, 415-16, Pseudoenergetic positive ions in plasma jets.
III. Acceleration of Charged Particles. Accelerators
Zhur. tekhn. fiz., 33, No. 3 (1963)
V. K. Grishin, 307-16, Interaction between a space charge and the high-frequency field in cyclic accelerators.
G. I. Zhileiko, 317-19, Effect of current of accelerated electrons on the propagation constant of a traveling
accelerating wave.
V. P. Bykov, 337-44, Effect of magnetic field inhomogeneities on particle. motion in a microtron.
Declassified and Approved For Release 2013/02/25: CIA-RDP10-02196R000600110001-6
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A. I. Pavlovskii, et al., 374-76, Note on the injection energy dependence of betatron intensity.
Pribory i tekhn. e'ksp., No. 1 (1963)
G. M. Anisimov and V. A. Teplyakov, 21-22, Focusing with an accelerating field.
Atomwirtschaft, 8, No. 2 (1963)
N. Hom, 99-100, The linear accelerator at the Riso research center.
Plasma Phys., 4, No. 6 (1962)
L. Sipek, 417-18, Stabilization of excitation of a betatron or synchrotron magnet.
IV. Nuclear Engineering. Nuclear Power
(Neutron physics. Nuclear reactor theory and calculations. Nuclear reactor design. Performance of nuclear reactors
and nuclear power stations. Radiation shielding. Disposal of radioactive wastes.)
Avto,matika i telemekh. (Mock. inzh. fiz. inst.), No. 3 (1962)
Yu. I. Gribanov, et al., 5-15, Test stand for nuclear plant power transients.
Yu. V. Grigor'ev and B. A. Kuvshinnikov, 16-21, Pulsed control of reactor power.
P. I. Popov and V. G. Terent'ev, 22-25, Enhanced reliability of a shielding system in the presence of noise.
Voprosy dozimetrii i zashchity of izluchenii, No. 1 (1962)
N. G. Gusev, et al., 7-23, Improved gamma-constant radioisotopes.
V. P. Mashkovich, 24-32, Use of point and slab directed sources in shielding materials studies.
V. I. Popov, 33-36, Note on self-absorption of gamma radiation in extended sources.
V. I. Popov, 37-45, Some experimental data on emission by cylindrical sources.
D. P. Osanov, 46-52, Contribution of emission resulting from multiple scattering in a volume source to the
dose. on the other side of the-shielding.
D. P. Osanov and E. E. Kovalev, 53-54, Determination of buildup factor of scattered emission from extended
sources.
A. V. Larichev and V. I. Mitin, 55-56, Buildup factors for low-energy gamma dosage in aluminum.
A. E. Kramer-Ageev and V. P. Mashkovich, 57-65, Dose distribution of fission neutrons in some shielding
media.
A. V. Larichev, et al., 66-73, Effect of channels in the shielding on attenuation of gamma emission from ex-
tended sources.
A. M. Panchenko, 74-77, Use of standard dosimeters in fields of pulsed gamma radiation.
V. V. Pavlov, 78-80, Note on the use of the Sakharov counter in an abruptly varying gamma field.
Sbornik trud. Mosk. inzh.-stroit. inst. im. Kuibysheva, No. 41 (1962)
S. T. Shershnev, 21-32, Nuclear reactor safety and strength evaluation of containment sheels.
L. N. Zaitsev and M. M. Komochkov, 33-44, Optimum amount of water in concrete reactor shielding.
Teploenergetika, No. 2 (1963)
L. S. Sterman and V. D. Mikhailov, 82-87, Determination of burnout in boiling of high-boiling coolant in
pipes.
Trudy nauchno-issled. inst. betona i zhelezobetona akad. stroit. i arkhitekt. SSSR, No. 29 (1962)
A. E. Desov and V. I. Nodol'skii, 4-36, Some aspects of heavy concrete technology for radiation shielding.
Atomic Energy Review(IAEA), 1, No. 1 (1963)
E. Proksch, 5-42, Purification of reactor moderators and coolants.
Atomkernenergie, 8, No. 2 (1963) -
E. Kern, 41-51, Effect of reflector on reactor temperature coefficients.
Declassified and Approved For Release 2013/02/25: CIA-RDP1O-02196ROO0600110001-6
Declassified and Approved For Release 2013/02/25: CIA-RDP1O-02196ROO0600110001-6
A. Jannussis, 52-53, Thermal spectrum. in absorbing media.
H. Brauer, 54-61, Heat transfer in annular gaps by forced convection and local boiling (II).
H. Weiss, 70-73, Measurement of reactor pulse power by Cherenkov radiation.
A tompraxis. 9, No. 2 (1963)
Beauge, et al., 52-58, French reactors for studying'biological shielding.
F. Reiff, et al., 52-58, Deactivation of tissues with polyphosphate solutions.
H. Bernhardt, 64-67, Study of deactivating action of a filter unit.
Atomwirtschaft, 8, No. 2 (1963)
--, 48-50, Outlook for nuclear power development in the Scandinavian countries.
.H. Brynielsson, 51-54, Nuclear power in Sweden.
0. Gimstedt and I. Wivstad, 55-57, Introduction of nuclear electric power generating stations to the Swedish
electric power grid.
C. Mileikowsky, et al., 58-62, The Swedish atomic industry.
P. Margen, 63-67, Development of reactor design in Sweden.
E. Laurila, 78-89, Development of nuclear power in Finland.
T. Bjerge, 80-83, The Danish Atomic Energy Commission and the Riso Research Center.
H. Harboe, 84-87, Danish power picture and the Danish nuclear industry program.
S. Werner, 87-88, Nuclear maritime reactor projects in Denmark.
A. Jonsson, 105-108, Pressurized heavy-water reactor and uniform fuel placement.
C. Jacobsen, 112, The Riso plant for processing low-level liquid wastes.
G. Randers, 117-118, Atomic energy in Norway.
F. Moller, 119-120, Norwegian industry and nuclear power.
T. Volledal, 121-22, The Norwegian Atomic Energy Institute.
R. Rose. 123-26, The Halden heavy-water boiling reactor.
V. Eriksen, 127029, The reactor physics research program at the NORA reactor in Norway.
J. Wilhelmsen, 130-32, Development of nuclear seagoing power plants in Norway.
Chem. and Process Engng., 44, No. 3 (1963)
T. Deighton, 138-44, Development of water-moderated reactors.
Energie nucl6aire, 5, No. 1 (1963)
W. Haegi, 26-30, Processing of radioactive wastes and uranium recovery.
Y. Prax, 35-39, The Mol nuclear energy research reactor.
Engineer, 215, No. 5587 (1963)
-, 336-40, Nuclear merchant ship reactor project.
--, 382-84, Present and future costs for large-scale nuclear power stations,
Engineer, 215, No. 5588 (1963)
--, 400-401, Heavy-water steam-generating reactor.
Engineer, 215, No. 5590 (1963)
--, 468-472, Evaluation of gas-cooled reactors.
Engineer, 215, No. 5591 (1963)
--, 509-511, Improved gas-cooled reactor No. 1 at Windscale.
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--, 545-48, Core characteristics of the Yankee power station reactor.
Engineer, 215, No. 5592 (1963),
--, 554-58, Commissioning and performance of the AGR reactor at Windscale.
-, 579-582, The improved gas-cooled reactor at Windscale.
Industries Atomiques, 7, No. 1-2 (1963)
R. Darras, 55-65, Corrosive attack on zirconium and zirconium alloys by high-temperature gases.
L. M. Vincent, et al., 67-77, 79-80, Corrosive attack on zirconium and zirconium alloys by uranium hexa-
fluoride.
Kernenergie, 5, No. 2 (1963)
G. Bessner, et al., 55-63, Calculation of effective cross sections for uranium-water lattices.
Kemtechnik, 5, No. 2 (1963)
H. Fendler, et al., 41-54, Determination of radiation conditions and effectiveness of biological shielding at
the inauguration of the Kahl nuclear reactor power stations.
W. Ullrich, 54-61, Fabrication, assembly, and testing of the main components of the Kahl nuclear reactor
power stations.
R. Hemmleb, 62-63, Experience in the construction of the Kahl nuclear reactor power stations.
D. Ulken, 63-65, Heat transfer test stand for maritime reactor components.
H. Muller and H. Uschwa, 66-71, Heat removal system in the DRAGON high-temperature reactor.
H. Acher, 71-75, Development of control rod drives for boiling-water reactors.
B. Schallopp. 76-79, Survey of reactivity measurement techniques.
Nucl. Energy (March, 1963)
P. Egelstaff, 66-69, Scattering of subthermal neutrons by metals.
Nucl. Engng., 8, No. 83 (1963)
--, 115-21, Evaluation of the AGR improved gas-cooled reactor.
G. Hefferon, 122-26, Reliability of a nuclear power station.
127-32, Nuclear power on the line in Sweden.
Nucl. Power, 8, No. 83 (1963)
B. Aler, 34-36, Nuclear power picture in Sweden.
P. Margen, 37-39, The Swedish Marviken nuclear reactor power station project, around a boiling heavy-water
reactor.
N. Rydell, 40-42, The Swedish Agesta power station.
0. Hellstrom, 42-44, Reactor pressure vessel (Agesta).
T. Wykman, 44-46, Heat exchangers (Agesta).
P. Erdhall, 47-48, Fuel transfer mechanisms (Agesta).
S. Ericsson, et al., 48-50, Control equipment (Agesta).
0. Hedstrom, 51-53, Installation and assembly of Agesta components.
Nucl. Power, 8, No. 84 (1963)
R. Coombe, 54-56, Neutron energy spectra. III. Measurements in the 0.5-15 MeV energy range.
R. Guard, 51-53, Status of reactor design as of 1962.
A. Wyatt, 57-60, The CANDU reactor and the Canadian power reactor building program.
Declassified and Approved For Release 2013/02/25: CIA-RDP1O-02196ROO0600110001-6
Declassified and Approved For Release 2013/02/25: CIA-RDP1O-02196ROO0600110001-6
Nucleonics, 21, No. 4 (1963)
--, 47-52, Reactors on the lines: Indian Point.
D. Harvey, et al., 56-59, Reliability and safety of isotope generator for space missions.
C. Heindl, et al., 80-85, Fission-fragment conversion reactors for space.
Nukleonik, 5, No. 2 (1963)
T. Gozani, 55-62, The reactivity concept and its application to kinetic measurements.
A. Fraude, 62-67, On the solution of kinetics equations for the case of periodic reactivity variations.
C. Hashmi, 67-74, Absorption of energy, transmission, and diffusion of gamma radiation in infinite homogen-
eous media.
D. Emendorfer, 74-82, Boundary conditions for neutron flow in a cylinder of finite dimensions, according to
the PL-approximation of the transport equation.
H. Kellner, 85-86, An attempt on an explicit derivation of the Boltzmann equation.
V. Nuclear Materials
(Geology. Chemistry. Chemical technology. Metallurgy)
Vestnik Leningrad. Univ., No. 24, Seriya geol. i geograf., No. 4 (1962)
L. F. Syritso, 65-73, Data on uraniferous minerals from one of the pegmatitic deposits.
Doklady akad. nauk SSSR, 147, No. 5 (1962)
N. I. Blinova, et al., 1112-13, On the magnetic properties of U205.
Doklady akad. nauk SSSR, 147, No. 6 (1962)
A. V. Nikolaev and Yu. A. Afanas'ev, 1380-81, Mutual effects of thorium nitrate and cerium nitrate (IV) in
coextraction by tributylphosphate.
Zhur. anal. khim., 17, No. 9 (1962)
I. A. Berezin and V. I. Malyshev, 1101-1104, Determination of trace amounts of hydrogen and oxygen in
uranium metal.
Zhur. strukturn. khim., 3, No. 6 (1962)
A. V. Karyakin and M. P. Volynets, 714-16, Infrared spectra of thorium carbonate complex.
M. E. Dyatkina and Yu. N. Mikhailov, 724-47, Structure of uranyl and its analogs.
Zhur. fiz. khim., 36, No. 11 (1962)
E. D. Kiseleva, et al., 2457-64. Investigation of the radiation stability of ion exchange resins.
E. D. Kiseleva, et al., 2465-68,-Effect of ionizing radiations from a stream of accelerated electrons on anion
exchange resins.
Izvestiya akad. nauk SSSR, Otdel. tekhn. nauk. Metallurgiya i toplivo, No. 6 (1962)
I. N. Plaksin, et al., 185-91, Extraction of rare earths.
Atomic Energy Revue (IAEA), 1, No. 1 (1963)
S. Bush, 43-92, Special materials used in reactor building and their. fabrication technology.
Atomwirtschaft, 8, No. 2 (1963)
L. Hall and S. Brandberg, 101-104. Fabrication of powder from sintered uranium dioxide.
S. Aas, 113-16, Nuclear fuel and reactor materials in Norway.
Chem. and Process Engng., 44, No. 3 (1963)
N. Hassett, 127-31, Areas of application of fluidization (review of patents granted).
L`nergie nuclMaire, 5, No. 1 (1963)
J. Doumerc, 4-15, Production technology of fuel elements.
P. Faugeras and M. Bourgeois, 16-25, Study of corrosion of uranium oxides and alloys in the gaseous phase,
with applications to spent fuel elements.
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Industries Atomiques, 7, No. 1-2 (1963)
A. Degeilh and R. Simon, 81-85, Defects in solids bombarded by charged particles. II.
Kernenergie, 5, No. 2 (1963)
S. T. Konobeevsky, 49-55, Present status of knowledge on the nature of radiation damage.
D. Naumann, 73-76, Laboratory investigation of recovery of uranium fuel by the chlorination method.
D. Naumann, 81, Ion exchange separation of plutonium on SBW wofatite in an alcoholic solution of hydro-
chloric acid.
Nature, 197, No. 4873 (1963)
P. Pauson, et al., 1200, Acid leaching of uranium and thorium carbides.
Nucl. Power, 8, No. 83 (1963)
--, 54-55, The Ronstad uranium mill.
Nukleonik, 5, No. 2 (1963)
C. Keller, 41-48, Investigation of germanates and silicates of tetravalent elements from thorium to ameri-
cium.
H. Riedel, 48-54, Properties of inorganic ion exchange zirconium-base and clayey mineral resins.
VI. Dosimetry and Radiometry. Nuclear Meteorology
Voennyi med. zhur., No. 12 (1962)
I. S. Sobol', 36-37, Gamma shielding in calibration of dosimetric instrumentation.
Izvestiya akad. nauk SSSR, Seriya geofiz., No. 1 (1963)
K. P. Makhan'ko, 183-87, On the shape of the spectrum of particle sizes of radioactive dust of natural origin.
Trudy akad. nauk Litov. SSR, Seriya B., 4 (1962)
. B. I. Styro and C. A. Garbaliauskas, 23-40, On the natural radioactivity of atmospheric fallout and some re-
lated problems.
Atomkemenergie, 8, No. 2 (1963)
K. Becker, 74-77, Sources of error in neutron personnel dosimetry using nuclear emulsions.
G. Malkowski, 78-79, Arguments on the timely detection of radioactive fallout.
Atompraxis, 9, No. 2 (1963)
L. Distel, et al., 39-44, Practical aspects of the use of radiometers and pocket dosimeters.
H. Hardt, et al., 45-48, Dosimetry using phosphate glass.
Kernenergie, 5, No. 2 (1963)
M. Frank, 76-80, Thermoluminescent dosimetry using the LiF phosphor, and energy dependence of thermo-
luminescent dosimeters.
Nature, 197, No. 4871 (1963)
T. Mamuro, et al., 964-66, Fractionation of high-level fallout.
Nucleonics, 21, No. 4 (1963)
N. Baily and K. Hoalst, 68, 70, 72-73, Dosimetry of space radiations.
VII. Radioactive and Stable Isotopes
(Separation, production, use)
Pribory i tekhnika eksp., No. 1 (1963)
Yu. S. Zaslavskii, et al., 149-52, Measurement of coating thickness by recording scattered betas.
Soobshch. akad. nauk Gruz. SSR, 29, No. 6 (1962)
I. N. Pantskhava, 691-95, Note on the use of radioisotopes to determine the physicomechanical properties
of concrete.
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Declassified and Approved For Release 2013/02/25: CIA-RDP1O-02196ROO0600110001-6
Atomic Energy Review, 1, No. 1 (1963)
R. Hara, 93-140, Chemical research performed at nuclear research reactors.
Atomwirtschaft, 8, No. 2 (1963)
C. Osterlundh and L. Erwall, 67, 68, 73, 74, Production and use of radioactive isotopes in Sweden.
K. Heydorn, 93-95, Production of radioactive isotopes in Denmark.
E. Somer, 96-98, Technical applications of radioactive isotopes in Denmark.
U. Been, 133-135, Fabrication and use of radioactive isotopes in Norway.
Energie nucl6aire, 5, No. 1 (1963)
A. Loverdo, 31-34, Process control instruments and processes utilizing trace isotopes.
JadernS Energie, No. 6 (1963)
F. Behounek, K. Barta, and B. Fiser, Rapid monitoring of beta activity in liquid wastes.
J. Silar and O. Novakova, Single-crystal scintillation gamma spectrometer: parameters and applications.
K. Stetina, Cermets: a material for fuel element cladding.
L. Simon, Use of radioactive traces in coal flotation.
J. Boucek, High-voltage source for radiation detectors.
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Soviet Journals Available in Cover-to-Cover Translation
ABBREVIATION
RUSSIAN TITLE
AE
Atomnaya energiya
Soviet Journal of Atomic Energy
Consultants Bureau
Akust. zh.
Akusticheskii zhurnal
Soviet Physics -'Acoustics
American Institute of Physics
Astronomicheskii zhurnal
Soviet Astronomy - AJ
American Institute of Physics
Astr(on). zh(urn).
Avtomaticheskaya svarka
Automatic Welding
Br. Welding Research Assn
(London)
Avto(mat). svarka
Avtomatika i Telemekhanika
Automation and Remote Control
.
Instrument Society of America
Biofizika
Biophysics
National Institutes of Health**
Biokhimiya
Biochemistry
Consultants Bureau
Byull. eksp(erim).
Byulleten' eksperimental'noi
Bulletin of Experimental
Consultants Bureau
biol. (i med.)
biologii 1 meditsiny
Biology and Medicine
DAN (SSSR)
Doklady) AN SSSR
Doklady Akademii
Nauk SSSR
Life
Sciences
Chemical
Sciences
Earth
Sciences
theory of elasticity sections)
Doklady Biological Sciences Sections National Science Foundation-
(includes: Anatomy, biochemistry, biophysics,
cytology, ecology, embryology,
endocrinology, evolutionary morphology,
genetics, histology, hydrobiology,
microbiology, morphology, parasitology,
physiology, zoology)
Doklady Botanical Sciences Sections
(includes: Botany, phytopathology,
plant anatomy, plant ecology, emb plant morphology)plant physiology,
j Proceedings of the Academy of Sciences
Proceedings of the Academy of Sciences
of the USSR, Section: Chemistry
Proceedings of the Academy of Sciences
of the USSR, Section: Physical Chemistry
Doklady Earth Sciences Sections
(includes: Geochemistry, geology,
geophysics, hydrogeology, lithology,
mineralogy, oceanology, paleontology,
permafrost, petrography)
Proceedings of the Academy of Sciences
of the USSR, Section: Geochemistry
Proceedings of the Academy of Sciences
f
o
th
USSR
e
Section: Geology
,
Soviet Mathematics - Doklady
Soviet Physics - Doklady
(includes: Aerodynamics, astronomy,
Consultants Bureau
American Geological Institute
Consultants Bureau
American Mathematical Society
American Institute of Physics
crystallography, cybernetics and control
theory, electrical engineering, energetics,
fluid mechanics, heat engineering,
hydraulics, mathematical physics,
mechanics, physics, technical physics,
Elektrosvyaz'
Telecommunications
Am. Inst. of Electrical Engineers
EntQm(ol). oboz(r).
Entomologicheskoe obozrenie
Entomological Review
National Science Foundatio
**
FMM
Fizika metallov i metallovedenie
Physics of Metals and Metallography
n
Acta Metallurgica
FTT, Fiz. tv(erd). tela
Fizika tverdogo tela
Soviet Physics - Solid State
American Institute of Physics
Fiziol. Zh(um). SSSR
Fiziologicheskii zhurnal imeni
Sechenov Physiological Journal USSR
National Institutes of Health**
I.M. Sechenov
Fiziol(ogiya) rast.
Fiziologiya rastenii
Plant Physiology
National Science Foundation*
Geodeziya i aerofotosyemka
Geodesy and Aerophotography
American Geophysical Union
Geokhimiya
Geochemistry
The Geochemical Society
Geol. nefti i gaza
Geologiya nefti i gaza
Petroleum Geology
Petroleum Geology
Geomagnetizm i aeronomiya
Geomagnetism and Aeronomy
American Geophysical Union
Iskusstvennye sputniki zemli
Artificial Earth Satellites
Consultants Bureau
Izmerit. tekhn(ika)
Izmeritel'naya tekhnika
Measurement Techniques
Instrument Society of America
TRANSLATION BEGAN
Vol. Issue Year
1
1
34 .
12
27
6
21
41
1
1
1
1
1
1
1
1
1956
1955
1957
1959
1956
1961
1956
1959
106
1
1956
106
1
1956
112
1
1957
124
1
1959
106-
1
1956-
123
6
1958
112-
1
1957-
123
6
1958
130
1
1960
106
1
1956
1
1957
37
1
1958
5
1
1957
1
1
1959
47
1
1961
4
1
1957
1962
2
1
1958
1
1
1961
1
1
1958
7
1
1958
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Izv. AN SSSR
O(td). Kh(im). N(auk)
Izv. AN SSSR
O(td). T(ekhn). N(auk):
Metall). i top.
Izv. AN SSSR Ser. fiz(ich).
Izv. AN SSSR Ser. geofiz.
Izv. AN SSSR Ser. geol.
Iz. Vyssh. Uch. Zav.,
Tekh. Teks. Prom.
Kolloidn. zh(urn).
Metallov. i term.
Met. i top.(gorn.)
Mikrobiol.
OS, Opt. i spektr.
Paleontol. Zh(urn)
Pribory i tekhn.
oks(perimenta)
Priki. matem. i mekh(an).
PTE
Radiotekh.
Radiotekhn. i elektron(ika)
Stek. i keram.
Svaroch. proiz-vo
Teor. veroyat. i prim.
Tsvet. metally
UFN
UKh, Usp. khimi
UMN
Vest. mashinostroeniya
Vop. onk(ol).
Zav(odsk). lab(bratoriya)-
ZhAKh, Zh. anal(it). Khim(ii`
ZhETF
Zh. dksperim. i teor. fiz.
ZhFKh
Zh. fiz. khimii
ZhNKh
Zh. neorg(an). khim.
ZhOKh
Zh. obshch. khim.
ZhPKh
Zh. prikl. khim.
ZhSKh
7
Bulletin of the Academy of Sciences of
the USSR: Division of Chemical Science
Bulletin of the Academy of Sciences
of the USSR: Physical Series
Bulletin of the Academy of Sciences
of the USSR: Geophysics Series . '
Bulletin of the Academy of Sciences
of the USSR: Geologic Series
Technology of the Textile Industry, USSR
Soviet Rubber Technology
Kinetics. and Catalysis
Coke and Chemistry, USSR
Colloid Journal
Soviet Physics - Crystallography
Metals Science and Heat Treatment of
Metals '
Metallurgist
Russian Metallurgy and Fuels(mining)
Microbiology
Refractories
Optics and Spectroscopy
Journal of. Paleontology
Soviet Soil Science
Soviet Powder Metallury and Metal Ceramics
Instrument Construction
Instruments and Experimental Techniques
Applied Mathematics and Mechanics
Problems of the North
Radiochemistry
Radio Engineering
Radio Engineering and Electronic Physics
Stal (in English)
Machines and Tooling
Glass and Ceramics
Welding Production
Theory of Probability and Its Application
The Soviet Journal of Nonferrous Metals
Soviet Physics - Uspekhi (partial translation)
Russian Chemical Reviews
Russian Mathematical Surveys
Russian Engineering Journal
Problems of Oncology
Industrial Laboratory
Journal of Analytical Chemistry
'Soviet Physics - JETP
Russian Journal of Physical Chemistry
Journal of Inorganic Chemistry
Journal of General Chemistry USSR,
Journal of Applied Chemistry USSR,
I
Zh. strukt(urnoi) khim.
ZhTF
Zh. tekhn. fiz.
Zh. vyssh. nervn. deyat.
(im. Pavlova)
Izvestiya Akademii Nauk SSSR:
Otdelenie khimicheskikh nauk
(see Met. i top)
Izvestiya Akademii Nauk SSSR:
Seriya fizicheskaya
Izvestiya Akademii Nauk SSSR:
Seriya geofizicheskaya
Izvestiya Akademii Nauk SSSR:
Seriya geologicheskaya
Izvestiya Vysshikh Uchebnykh Zavedenii
Tekhnologiya Tekstil'noi
Promyshlennosti
Kauchuk i rezina
Kinetika i kataliz
Koks i khimiya
Kolloidnyi zhurnal
Kristallografiya
Metallovedenie i termicheskaya
obrabotka metallov
Metallurg
Metallurgiya i toplivo (gornoye delo)
Mikrobiologiya
Ogneupory
Optika i spektroskopiya
Paleontologicheskii Zhurnal
Pochvovedenie
Poroshkovaya Metallurgiya
Pribory i.tekhnika a ksperimenta
Prikladnaya matematika'i mekhanika
(see Pribory i tekhn.'eks.)
Problemy Severa
Radiokhimiya
Radioteknika
Radiotekhnika i electronika
Stal'
Stanki i instrument
Steklo i keramika
Svarochnoe proizvodstvo
Teoriya veroyatnostei i ee primenenie
Tsvetnye metally.
Uspekhi fizicheskikh nauk
Uspekhi khimii
Uspekhi matematicheskaya nauk
Vestnik mashinostroeniya
Voprosy onkologii
Zavodskaya laboratoriya
Zhurnal analiticheskoi khimii
Zhurnal eksperimental'noi i
teoreticheskoi fiziki
Zhurnal fizicheskoi khimii
Zhurnal neorganicheskoi khimii
Zhurnal obshchei khimii
Zhurnal prikladnoi khimii
Zhurnal strukturnoi khimii
Zhurnal tekhnicheskoi fiziki
Zhurnal vychislitel'noi matematika i
maternaticheskoi fiziki
Zhurnal vysshei nervnoi
deyatel'nosti (im I. P. Pavlova)
*Sponsoring organization. Translation published by Consultants Bureau.
**Sponsoring organization. Trarislation published by Scripta Technica.
Journal of Structural Chemistry
Soviet Physics - Technical Physics
U.S.S.R. Computational Mathematics and
Mathematical Physics
Columbia Technical Translations,
18
3
1954
American Geophysical Union
7
1
1957
American Geological Institute
23
1
1958
The Textile Institute (Manchester)
4
1
1960
Palmerton Publishing Company, Inc.
18
3
1959
Consultants Bureau
1
1
1960
Coal Tar Research Assn. (Leeds, England)
8
1959
Consultants Bureau
14
1
1952
American Institute of Physics
2
1
1957
Acta Metallurgica
6
1
1958
Acta Metallurgica
1
1957
Scientific Information Consultants, Ltd.
1
1960
National Science Foundation*
26
1
1957
Acta Metallurgica
25
1
1960
American Institute of Physics
6
1
1959
American Geological Institute
1
1962
National Science Foundation**
53
1
1958
Consultants Bureau
2
1
1962
Taylor and Francis, Ltd. (London)
4
1
1959
Instrument Society of America .
3
1
1958
Am. Society of Mechanical Engineers
22
1
1958
National Research Council of Canada
1
1958
Consultants Bureau
4
1
19.62
Am. Instifute of Electrical Engineers
16
1
1961
A'm. Institute of Electrical Engineers
6
1
1961
Iron and Steel Institute
19
1
1959
Production Engineering Research Assoc.
30
1
1959
Consultants Bureau
13
1
1956
Br. Welding Research Assn. (London)
5
4
1959
Soc. for Industrial and Applied Math.
1
1
1956
Primary Sources
33
1
1960
American Institute of Physics
66
1
1958
Chemical Society (London)
29
1
1960
Cleaver-Hume Press, Ltd. (London)
15
1
1960
Production Engineering Research Assoc.
39
4
1959
National Institutes of Health**
7
1
1961
Instrument Society of America
24
1
1958
Consultants Bureau
7
1
1952
American Institute of Physics
28
1
1955
Chemical Society (London)
33
7-
1959
Chemical Society (London)
4
1
1959
Consultants Bureau
19
1
1949
Consultants Bureau
23
1
1950
Consultants Bureau,
1
1
1960
American Institute of Physics
26
1
1956
Pergamon Press, Inc. .
1
1
1962
National Institutes of Health**
11
1
1961
Declassified and Approved For Release 2013/02/25: CIA-RDP10-02196R000600110001-6
Declassified and Approved For Release 2013/02/25: CIA-RDP10-02196R000600110001-6
SIGNIFICANCE OF ABBREVIATIONS MOST FREQUENTLY
ENCOUNTERED IN SOVIET PERIODICALS
FLAN
GDI
GITI
GITTL
GONTI
Gosenergoizdat
Goskhimi zdat'
GOST
GTTI
IL
ISN (Izd. Sov. Nauk)
Izd. AN SSSR
Izd. MGU
LEIIZhT
LET
LETI
LETIIZhT
Mashgiz
MEP
MES
M ES EP
MGU
MKhTI
MOPI
MSP
NI ZVUKSZAPIOI
NIKFI
ONTI
OTI
OTN
Stroiizdat
TOE
TsKTI
TsNIEL
TsNIEL-MES
TsVTI
UF
VIESKh
VNIIM
VNIIZhDT
VTI
VZEI
Phys. Inst. Acad. Sci. USSR.
Water Power Inst.
State Sci.-Tech. Press
State Tech. and Theor. Lit. Press
State United Sci.-Tech. Press
State Power Press
State Chem. Press
All-Union State Standard
State Tech. and Theor. Lit. Press
Foreign Lit. Press
Soviet Science Press
Acad. Sci. USSR Press
Moscow State Univ. Press
Leningrad Power Inst. of Railroad Engineering
Leningrad Elec. Engr. School
Leningrad Electrotechnical Inst.
Leningrad Electrical Engineering Research Inst. of Railroad Engr.
State Sci. -Tech. Press for Machine Construction Lit.
Ministry of Electrical Industry
Ministry of Electrical Power Plants
Ministry of Electrical Power Plants and the Electrical Industry
Moscow State Univ.
Moscow Inst. Chem. Tech.
Moscow Regional Pedagogical Inst.
Ministry of Industrial Construction
Scientific Research Inst. of Sound Recording
Sci. Inst. of Modern Motion Picture Photography
United Sci.-Tech. Press
Division of Technical Information
Div. Tech. Sci.
Construction Press
Association of Power Engineers
Central Research Inst. for Boilers and Turbines
Central Scientific Research Elec. Engr. Lab.
Central Scientific Research Elec. Engr. Lab.-Ministry of Electric Power Plants
Central Office of Economic Information
Ural Branch
All-Union Inst. of Rural Elec. Power Stations
All-Union Scientific Research Inst. of Metrology,
All-Union Scientific Research Inst. of Railroad Engineering
All-Union Thermotech. Inst.
All-Union Power Correspondence Inst.
Note: Abbreviations not on this list and not explained in the translation have been transliterated, no further
information about their significance being available to us. -Publisher.
Declassified and Approved For Release 2013/02/25: CIA-RDP10-02196R000600110001-6
Declassified and Approved For Release 2013/02/25: CIA-RDP10-02196R000600110001-6
SOVIET
RADIOCHEMISTRY
(RADIOKHIMIYA)
In cover-to-cover translation
A new Soviet journal (first issued in 1959) publishes
research works emanating from the Khlopin Radium In-
stitute, Academy of Sciences USSR, and is under the
editorial supervision of Academician V. M. Vdovenko,
director of the Institute. The other members of the edito-
rial board include such top researchers as I.P. Alimarin,
A. I. Brodskii, E. K. Gerling; A. A. Grinberg,` V. It. Klok-
man, L. V. Komlev, B. V. Kurchatov, A. N. Nesmeyanov,
A. V. Nikolaev, B. P. Nokol'skii, V. I. Spitsyn, I. E. Starik,
and A. P. Vinogradov.,,
In present-day science and technology, where the radio-
active properties of various substances are finding in-
creased application in the study of chemical reactions
and properties, it is of great importance that the Western
scientific community be cognizant of Soviet progress in
radiochemistry. The translations of SOVIET RADIOCHEM-
ISTRY will provide a running account of Soviet progress
in the chemistry of atomic elements, methods of research
in radiochemistry,, the study of radioactivity, the history
of radiochemistry, and applied radiochemistry. The in-
formation and letters section contains concise accounts
of interesting research in radioactivity!
Contributors to the journal include S. Z. Roginskii, `I. V.
Tananaev, P.I. Kondratov, A. D, Gel'man, Yu V. Egorov,
V. P. Zaitseva, V. P. Shvedov, A. N. Ponomarev, V. S.
Zlobin, and members of the editorial board.
The journal is issued bi-monthly, as will be the English
edition. Translation began with the first issue of 1962.
Study of Coprecipitation of Microimpurities in Iso-
thermal Relief of Supersaturation of a K2SO4 Solu-
tion. II..Coprecipitation of,Lanthanum with K2S04
Crystallization Coefficents of , Some Alkali-Metal
Halides with Microconcentrations of One of the Com-
ponents ? Coprecipitation of Microgram Amounts of
Molybdenum with Some Inorganic Precipitates
Temperature Dependence of Distribution Coefficents
in the Extraction of Uranyl Nitrate from Aqueous'
Solutions with Diethyl Ether ? Salting-Out Action of
Group 11 Metal Nitrates in the Extraction of Uranyl
Nitrate with Diethyl Ether ? Physicochemical Charac-
teristics of the.Dynamics of Sorption of Radioactive
Substances -.State of Protactinium in Aqueous Solu-
tions. VI. Adsorption, Properties of Protactinium
Sorption of Some Radioactive Isotopes from Aqueous
Solutions by Active Maganese Dioxide ? Adsorption
of Yttrium and Zirconium by Zirconium Phosphates
? Structure of Uranyl Nitrate Dihydrate ? Plutonium
Fluorides ? 'Hydrolytic Behavior of Plutonyl in
Aqueous Solutions Elution of Neptunium from
the Anionite AM ? Use of Ion Exchange\to Study
the State of a Substance in Solution. VIII. Study of
Uranyl Carbonate Solutions by Ion Exchange ? Chro-
matographic Separation of Protactinium from Zir-
conium, Titanium, and Niobium ? Chromatographic
Concentration of Astatine ? Isolation of a Group of
Carrier-Free`: Rare Earth Fission Products from
Uranium and Thorium ? Determination of Ms Thl by'
Ms Th1I /3-Particles in the Presence of Radium-226
Determination of Radioactive Cesium by the Ferro-'
cyanide Method ? Determination of Low Levels of
Radioactive Contaminants in Water Reaction of
Recoil Tritium Atoms with Benzene Recoil Effect
in Inner-Complex Compounds of Cobalt in the Re-
action C&9(n, 2n)Co-18 ? Yields of Spallation and Fis-'
sion Reactions Induced by High-Energy Particles
,Mechanism of Zirconium Extraction by Organophos-
phorus Compounds Effect of Structural. Factors on
the Thermodynamic Characteristics of the Extraction
of Salts of Basic Dyes ? Effect of the Amount of
Absorbed Ions in a Chromatography Column on the
Position-of a Peak on the Elution Curve ? Diffusion
of Strontium-90 in Soil and Sand.
Annual subscription (6 issues): $95.00
CONSULTANTS BUREAU .227 West 17 St., Never, York 11,. N. Y.
Declassified and Approved For Release 2013/02/25: CIA-RDP10-02196R000600110001-6
Declassified and Approved For Release 2013/02/25: CIA-RDP10-02196R000600110001-6
SOVIET MASER RESEARCH
Edited by. Academician D.V. Skobel'tsyn
Reports of four coordinated researches into-the theory and applications' ofrnasers for frequency
standards, Conducted at the P. N. Lebedev:P,hysics Institute under the guidance of Academician
A. M. Prokorov. Transactions (Trudy) No. 21. , ? A
A THEORETICAL STUDY OF THE FREQUENCY STABILITY OF A MASER
by
A
I
Oraevskii
.
.,
.
The article presents a general analysis of the functioning of a molecular generator or,
maser operating with a molecular beam of "sorted" molecules.. Effects of,external per-
turbations (pressure and magnetic field effects) are treated, and the problem of hyperfine 10
structure of. the emission line `is considered. Cases treated in detail are those of masers
.using inversion transitions in ammonia. Some comparisons between theoretical and experi-
mental, results are given for such cases.
INVESTIGATION ,OF"THE CHARACTERISTICS ,OF MASERS
{1 ='3, K = 3 in ammonia N14H3)
by -M. Strakhovskii and I. V. Cheremiskii
Th authors report experimental Investigations into the dependence'Af frequency iand relax-,%
tive power of an ammonium maser, N16H,, on the'natural frequency of the resonator, the
voltage applied to the quadrupole condenser (or to a circular separatibn system) and the`
ammonia pressure in the rolecular beam'source. Also reported on is the dependence of
frequency and relative power of a'maser with two intersecting beams on ammonia pressure
in the molecular beam source.
THEORY OF THE HYPERFINE STRUCTURE
OF THE ROTATIONAL SPECTRA OF MOLECULES
by K. K. Svidzinskii ` -
A-theory of the hfs has been developed which allows the calculation of hyperfine effects
in rotational spectra of molecules (in a nondegenerate electronic ground state) With an
accuracy not lower than 10 cps. By applying methods of group theory, especially the
apparatus of irreducible tensor operators and the 3nj-symbols, 'the. calculation of hfs
has been successfully simplified and standardized.
In order to provide the necessary accuracy (not lower than-10 cps),-the present, treatment
includes, besides the usual dipole and-quadrupole interactions, the magnetic octupole,and
the electric hexadecapole interactions. A general calculation of the energy bf the spin-spin
interactions of nuclei in a rotating molecule is presented, along with a,general expression
for the energy of ,the dipole I.1 interaction in the asymmetric-top molecule. .
THE W MASER
by N. G. Basov,`V. S.1uev, and K. K. Svidzinskii ?
Reports work aimed at investigating the possibility of making a maser using inversion,
transitions of heavy ammonia NO;,` including the accomplishment of a working, model. The
.power output of the NO3 maser is reported as1i0'" watt at 1656.18 me ? f.~6, K=6 line
.in the inversion spectrum of ND,). The absolute stability of the, line, according to'pre-
liminary data, is of the order of 10-0.
.The results of calculations on the hyperfine inversion spectrum of ND, are given. Analysis
of the hyperfine structure leads to an estimate, for the absolute stability, of .the J=6,
K=6 line
SOVIET MASER RESEARCH contains a unique bibliography of all work performed' in the Laboratory
of Oscillations" FIAN, P. N. Lebede~ Institute from. 1935-1961, and covers topics such as..
Electron paramagnetic resonance; Quantum electronics; Molecular ` generators and amplifiers;'
Time standards; Gas radiospectroscopy; ;Propagation of radio waves; Statistical radiophysics;
Accelerators; and various other problems. /
Over 200 pages ' ? Translated from Russian $27.50
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