appraisement of the correction factors for neutron reaction in the manganese bath using monte carlo...
TRANSCRIPT
Appraisement of the correction factors for neutron reactionin the manganese bath using Monte Carlo calculation
Rahim Khabaz
Received: 17 October 2011 / Published online: 26 April 2012
� Akademiai Kiado, Budapest, Hungary 2012
Abstract In this work, the Monte Carlo method has been
used to simulate the manganese sulfate bath calibration
system, in order to evaluate the different interaction of
neutron with all nuclei of the components of the solution,
i.e., hydrogen, manganese, sulfur, and oxygen nuclei for241Am–Be and 252Cf neutron sources. Also, the leakage
probability of neutron has been calculated for various
radiuses of spherical bath containing a solution with weight
concentration of 93.68 g/(kg of solution). The simulations
performed by MCNPX, included a detailed description of
the geometry and material of the system (tank, holder and
source). The calculations were evaluated using neutron
cross sections from several libraries. The results of calcu-
lation show that the proper radiuses of spherical manganese
bath with this concentration, for 252Cf and 241Am–Be
sources, are about 35 and 60–65 cm, respectively.
Keywords Manganese bath � Neutron source � Correction
factor � Monte Carlo method
Introduction
In recent years, using the radio-isotopic neutron sources
have increased, so having knowledge such as their neutron
emission rate and energy spectrum are essential [1, 2]. The
manganese sulfate (MnSO4) bath technique is a widely
used method for the absolute determination of the neutron
emission rate of radio-isotopic neutron sources [3]. The
method consists of activating a solution of manganese
sulfate with a neutron source placed at the center of a
relatively large aqueous solution and inferring the strength
of the neutron source (Q) from the manganese activity of
the bath, by the 55Mn (n,c)56Mn reaction which has a half-
life of 2.5785 h [4].
The main capture reactions of fast neutrons are the type
(n,a), (n,d) and (n,p). In the solution of manganese sulfate,
the nuclei of the 16O and 32S often capture fast neutrons
through 16O(n,a)13C, 32S(n,a)29Si and 32S(n,p)32P reactions
and the other reactions is negligible compared to these [5].
The neutrons emitted from the source will be slowed
down, particularly through elastic scattering with hydrogen
nuclei. The created thermal neutrons are captured by the
nucleus produce reactions of type (n,c), which are likely to
occur for nearly all chemical elements (55Mn, 1H, 16O and32S). The thermal neutron-capture cross-section of oxygen
nuclei is negligibly small compared to those of the other
nuclei [5]. Neutron capture by hydrogen produces a stable
nucleus, a deuteron, and neutron capture by sulfur produces
a stable isotope, 33S. A fraction of the neutrons is absorbed
in manganese by (n,c) corresponds to the number of neu-
trons emitted from the neutron source. The c-rays of 56Mn
are counted with a NaI(Tl) scintillation detector at a well
shielded location by continuously pumping a fraction of the
MnSO4 solution to it.
For that activity to give the value of Q is necessary to
accomplish some types of corrections. The source strength,
Q, of the neutron source is obtained from the following
well known equation [6]:
Q ¼ RMn �1
f� 1e� 1
1� Ceð Þ 1� Csð Þ 1� Ccð Þ ð1Þ
where RMn—saturation count rate of the 56Mn measured by
the bath detector system, e—counting efficiency in NaI(Tl)
R. Khabaz (&)
Physics Department, Faculty of Sciences, Golestan University,
49138-15739 Gorgan, Iran
e-mail: [email protected]; [email protected]
123
J Radioanal Nucl Chem (2012) 293:455–462
DOI 10.1007/s10967-012-1792-0
detector which was fixed using 4pb–c coincidence
counting method [7], Ce—fractional neutron escape from
the boundaries of the bath, Cs—fraction of neutron
recaptured by the source and its mounting assembly,
Cc—fraction of neutron captured in the (n,p) and (n,a)
reactions by the nuclei of the components of the solution,
i.e., manganese, sulfur, and oxygen nuclei, f—fraction of
the remaining neutron captured by manganese in absence
of impurities in 55Mn(n,c)56Mn reaction:
1
f¼ 1þ rS
rMnð1þ G�rsÞMn
þ 4rO
rMnð1þ G�rsÞMn
þ NH
NMn
� rH þ 0:5rO
rMn 1þ G�rsð ÞMn
ð2Þ
where NMn, NH—concentrations of manganese and
hydrogen nuclei per cubic centimeter in the MnSO4 solu-
tion, rMn, rS, rH, rO—thermal neutron capture cross sec-
tions of manganese, sulfur, hydrogen and oxygen,
respectively.
The factor ð1þ G�rsÞ allows for the resonance capture in
manganese [8]. Indeed, in Eq. (2) the resonance capture
cross-section at the epithermal region for manganese nuclei
has been corrected by replacing the thermal neutron-cap-
ture cross-section rMn, with rMnð1þ G�rsÞ [9], where G is
the resonance self-shielding factor for the solution, �r: is a
spectral index averaged over the system and represents the
relative amount of the non-Maxwellian component of the
neutron energy distribution, and s is the resonance activa-
tion integral normalized to the thermal neutron-capture
cross section.
As discussed one method to determination of correction
factors for manganese sulfate bath is analytical solving the
Eqs. (1) and (2). By utilize the proper cross section of
different reaction for neutrons with various energies, the
correction factors can be given as a function of energy.
Because of the complication and using the approximation,
this process is not simple and accurate. As well as, the loss
regarding capture for the material of the source and
immersion system (Cs) cannot fix experimentally. Nowa-
days, with developed neutron transport and to the well-
evaluated nuclear cross-sections, individual evaluations of
the various correction factors can be abandoned and
replaced by a direct calculation of the probability of the
neutron capture by manganese nuclei, by using the Monte
Carlo method. The probability, PMn, of neutron absorption
by manganese nuclei in the actual bath with the actual
source can be directly calculated using an appropriate
Monte Carlo neutron transport code, e.g., MCNPX. Fur-
thermore, in this way, it is possible to consider quite easily
the energy spectrum of the source and the influence of all
construction materials. The source emission rate (Q) is then
given by the calculated probability PMn and the production
rate (RMn) of 56Mn by neutron capture,
Q ¼ 1
e� 1
PMn
� RMn ð3Þ
where by comparison between Eqs. (1) and (3) gives
1
PMn
¼ 1
f� 1
1� Ceð Þ 1� Csð Þ 1� Ccð Þ ð4Þ
In this work, the correction factors for neutron losses with
different process in all nuclei of solution are given for two
well-known sources, namely 241Am–Be and 252Cf by
Monte Carlo simulation included a detailed description of
the geometry and material using the MCNPX code. The
calculation was performed for various radiuses of spherical
bath, and suitable radius was determined for calibration of
each source. Consequently, one can acquire the neutron
rate of emission rate of the neutron source by experimental
measurement of the gamma emission rate of 56Mn in the
NaI(Tl) detector and using the calculated correction
factors.
Materials and methods
In this work the MCNPX Monte Carlo code with the
ENDF/B-VI.0, ENDF/B-V, ENDF/BVI.8 and ENDF/B-
VII.0 libraries was employed to calculate the correction
factors [10].
The geometry and the material composition of the bath
and the neutron source container were precisely described
in the MCNPX input file. The simulation was performed
for 241Am–Be and 252Cf neutron sources that their spec-
trum was extracted from the standard ISO 8529-1 [11]. The241Am–Be source was defined as a cylinder of beryllium
(with a density of 1.85 g/cm3) contained in a X.14 type
capsule with 60 mm in height and 30 mm in diameter. The
geometry 252Cf neutron source was modeled as a cylinder
of californium oxide (with a density of 15.10 g/cm3) filled
in a X.224 type capsule by dimensions of 32.5 mm in
length and 9.4 mm in outer diameter. The container cap-
sules of 241Am–Be and 252Cf sources constructed of 1.6
and 2.4 mm thickness of stainless steel (316L. type),
respectively.
The source was placed in a cylindrical Teflon (CnF2n?2)
holder (by density of 2.20 g/cm3) with 10 cm in height,
10 cm in diameter and 4.0 mm thickness. The inner space
of the Teflon container was assumed to be the air (with
density of 1.29 kg/m3 with elemental composition of
79.1 % N and 20.9 % O). This holder also was installed in
the center of a spherical tank which was had been filled
with an aqueous solution of pure MnSO4 (Fig. 1). The
container bath consisted of 3.0 mm thickness of stainless
steel (316L. type) with density of 7.93 g/cm3 whose ele-
mental composition was 1.000 % Si, 0.045 % P, 0.030 %
456 R. Khabaz
123
S, 0.030 % C, 17.000 % Cr, 65.395 % Fe, 12.000 % Ni,
2.000 % Mn and 2.5.000 % Mo (in terms of their weight
percentage in the composition) [12].
The set of bath used in this study consists of eight
stainless steel spherical tanks filled with manganese sulfate
solution. The weight concentration of MnSO4 in the solu-
tion was considered 93.68 g/(kg of Solution), and the
solution density was 1.0934 g/cm3 [13]. There are some of
the characteristics of the manganese baths simulated by
MCNPX in Table 1.
The number of each nuclear component of the solution
is deduced from the present concentration and density. The
concentrations of nuclei of the solution in units of nuclei/
barn-cm were 4.085 9 10-4 for manganese and sulfur, also
3.475 9 10-2 and 6.624 9 10-2 for oxygen and hydrogen,
respectively. Then the number ratio of hydrogen nuclei to
manganese nuclei was 162.15. The unusual ratio was
determined by the amount of high purity MnSO4 available
for the experiment. This ratio will be decreased as the
concentration increases.
Furthermore, it has been determined that the gamma
counting rate of the NaI(Tl) detector is increased with
decreasing the concentration of the solution [14]. This is
due to decreasing self-absorption of the 56Mn radiation as
the content of the solution decreases.
The calculation of the neutron capture for the solution,
source and immersion system was accomplished being
selected the tally F4 of MCNPX, being considered the
different reactions, associated to a card multiplier that
contains the volume of the solution, and the atom density
(atom/barn-cm) of the element (from Table 1) that interacts
for capture of neutrons. In the case of the leakage of
neutrons of the bath, this was estimated with the tally F1.
This tally was defined in a concentric external spherical
surface of the tank, and it represents the number of parti-
cles that cross the surface in any direction.
Result and discussion
Different reactions were calculated using Monte Carlo
MCNPX code for described geometry, material and sour-
ces. Indeed, (n,c), (n,p) and (n,a) reactions were evaluated
in all nuclei of MnSO4�H2O. The results of these calcula-
tions by using ENDF/B-VI.0 for the 241Am–Be and 252Cf
sources were given in Tables 2, 3, 4 and 5. It should be
noted that the calculations are normalized to one neutron of
source. The relative error (D) for each tally is listed in these
tables. The statistical errors in output of MCNPX for all
reactions, except 16O(n,p)16N, by the 241Am–Be and 252Cf
sources were less than 0.4 and 1 %, respectively. Also, for
recorded (n,p) reaction in 16O that has least probability and
very small amounts, relative error was under 6 %.
As it can be observed, for two sources in all radiuses the1H(n,c)2d reaction has a maximum probability compared to
other reactions. Considering the important role of the ratio
of NH/NMn in the solution, and the conditions of mea-
surement, the appropriate concentration of manganese
sulfate should be used. For oxygen nuclei, the dominant
reaction is (n,a), while this element has an insignificant
amount of thermal neutron capture by (n,c). In reaction of
fast neutrons with sulfur nuclei, (n,p) is dominant, as for241Am–Be source the ratio of S(n,p) to S(n,a) is about 1.90,
while for 252Cf source, this ratio is less and about 1.05. The
interaction of thermal neutrons with sulfur through32S(n,c)33S has the most contribution among the other
neutron interactions.
The most important reaction in calibration of neutron
source by manganese bath is 55Mn(n,c)56Mn. The proba-
bility of this reaction in different baths for 241Am–Be and
Fig. 1 Geometry of manganese bath in Monte Carlo simulation
Table 1 Some parameters of various manganese sulfate baths in
calculations
Tank no. Radius (cm) Volume (l) Mass of MnSO4 (kg)
1 35 1.787 9 102 18.173
2 40 2.672 9 102 27.171
3 45 3.808 9 102 38.724
4 50 5.227 9 102 53.153
5 55 6.960 9 102 70.776
6 60 9.039 9 102 91.914
7 65 1.149 9 103 116.884
8 70 1.436 9 103 146.008
Appraisement of the correction factors 457
123
252Cf source increases from 1.594 to 1.885 and 1.887 to
1.973 with increasing the radius, respectively. Although
other reactions such as (n,p) and (n,a) occur in manganese
nuclei, the probability of these reactions is negligible in
comparison to the (n,c) reaction. As well as, the correction
factors in Eqs. (1) and (2) were calculated for all
Table 2 Result of the MCNPX calculation by using ENDF/B-VI.0 for various radiuses of manganese bath (35, 40, 45 and 50 cm) with the241Am–Be source
Reaction r = 35 cm r = 40 cm r = 45 cm r = 50 cm
Probability D (%) Probability D (%) Probability D (%) Probability D (%)
H (n,c) 6.35E-01 0.09 6.81E-01 0.08 7.08E-01 0.07 7.28E-01 0.06
O (n,c) 1.91E-04 0.09 2.05E-04 0.08 2.13E-04 0.07 2.19E-04 0.06
O (n,p) 4.09E-06 3.10 4.20E-06 3.19 4.26E-06 3.24 4.22E-06 2.85
O (n,a) 3.87E-02 0.20 3.97E-02 0.20 4.02E-02 0.21 4.07E-02 0.18
S (n,c) 6.00E-03 0.09 6.44E-03 0.08 6.69E-03 0.07 6.87E-03 0.06
S (n,p) 1.35E-03 0.13 1.39E-03 0.14 1.41E-03 0.14 1.42E-03 0.13
S (n,a) 7.09E-04 0.10 7.31E-04 0.11 7.43E-04 0.11 7.53E-04 0.10
Mn (n,p) 3.30E-05 0.22 3.38E-05 0.23 3.42E-05 0.23 3.46E-05 0.21
Mn (n,a) 1.15E-05 0.31 1.17E-05 0.32 1.19E-05 0.33 1.20E-05 0.29
Cc 4.08E-02 3.13 4.19E-02 3.23 4.24E-02 3.28 4.29E-02 2.88
(1 - Cc)-1 1.04 0.13 1.04 0.14 1.04 0.15 1.05 0.13
Mn (n,c) 1.59E-01 0.09 1.71E-01 0.08 1.78E-01 0.07 1.83E-01 0.06
1/PMn 6.27 0.09 5.85 0.08 5.63 0.07 5.47 0.06
Leakage 1.52E-01 0.31 9.35E-02 0.40 5.72E-02 0.53 3.46E-02 0.6
(1 - Ce)-1 1.18 0.06 1.10 0.04 1.06 0.03 1.04 0.02
Source absorption 7.52E-03 4.13 7.65E-03 3.86 7.93E-03 3.81 8.05E-03 3.24
(1 - Cs)-1 1.01 0.03 1.01 0.03 1.01 0.03 1.01 0.03
The symbols are defined in the text
Table 3 Result of the MCNPX calculation by using ENDF/B-VI.0 for various radiuses of manganese bath (55, 60, 65 and 70 cm) with the241Am–Be source
Reaction r = 55 cm r = 60 cm r = 65 cm r = 70 cm
Probability D (%) Probability D (%) Probability D (%) Probability D (%)
H (n,c) 7.38E-01 0.05 7.45E-01 0.05 7.49E-01 0.05 7.51E-01 0.05
O (n,c) 2.22E-04 0.05 2.24E-04 0.05 2.25E-04 0.05 2.26E-04 0.05
O (n,p) 4.17E-06 2.29 4.19E-06 2.31 4.20E-06 2.33 4.21E-06 2.33
O (n,a) 4.09E-02 0.15 4.10E-02 0.15 4.11E-02 0.15 4.12E-02 0.15
S (n,c) 6.97E-03 0.05 7.03E-03 0.05 7.07E-03 0.05 7.09E-03 0.05
S (n,p) 1.43E-03 0.11 1.44E-03 0.11 1.44E-03 0.11 1.44E-03 0.11
S (n,a) 7.58E-04 0.08 7.61E-04 0.08 7.63E-04 0.08 7.64E-04 0.08
Mn (n,p) 3.48E-05 0.17 3.49E-05 0.17 3.50E-05 0.17 3.50E-05 0.17
Mn (n,a) 1.21E-05 0.24 1.21E-05 0.24 1.21E-05 0.24 1.21E-05 0.24
Cc 4.31E-02 2.32 4.33E-02 2.34 4.34E-02 2.36 4.34E-02 2.36
(1 - Cc)-1 1.05 0.11 1.05 0.11 1.05 0.11 1.05 0.11
Mn (n,c) 1.85E-01 0.05 1.87E-01 0.05 1.88E-01 0.05 1.88E-01 0.05
1/PMn 5.40 0.05 5.35 0.05 5.32 0.05 5.31 0.05
Leakage 2.09E-02 0.62 1.25E-02 0.81 7.51E-03 1.05 4.52E-03 1.34
(1 - Ce)-1 1.02 0.01 1.01 0.01 1.01 0.01 1.00 0.01
Source absorption 8.35E-03 3.12 8.86E-03 3.07 9.13E-03 3.07 9.51E-03 3.05
(1 - Cs)-1 1.01 0.03 1.01 0.03 1.01 0.03 1.01 0.03
The symbols are defined in the text
458 R. Khabaz
123
geometries. As it can be seen, the minimum deviation of
these from the ideal condition (i.e., if all neutrons are
thermalized and captured by the 55Mn nuclei) is for the
factor of neutron recaptured by the source and its mounting
assembly. By the both sources, the factor of leakage from
the bath boundaries has the maximum deviation for spheres
Table 4 Result of the MCNPX calculation by using ENDF/B-VI.0 for various radiuses of manganese bath (35, 40, 45 and 50 cm) with the 252Cf
source
Reaction r = 35 cm r = 40 cm r = 45 cm r = 50 cm
Probability D (%) Probability D (%) Probability D (%) Probability D (%)
H (n,c) 7.52E-01 0.07 7.69E-01 0.07 7.76E-01 0.06 7.82E-01 0.06
O (n,c) 2.26E-04 0.07 2.31E-04 0.07 2.33E-04 0.06 2.35E-04 0.06
O (n,p) 1.80E-05 5.59 1.87E-05 5.69 1.90E-05 5.78 1.94E-05 5.86
O (n,a) 5.66E-03 0.55 5.77E-03 0.56 5.82E-03 0.56 5.88E-03 0.57
S (n,c) 7.10E-03 0.07 7.26E-03 0.06 7.33E-03 0.06 7.38E-03 0.06
S (n,p) 3.14E-04 0.31 3.19E-04 0.32 3.21E-04 0.32 3.24E-04 0.33
S (n,a) 3.02E-04 0.18 3.06E-04 0.19 3.08E-04 0.19 3.10E-04 0.19
Mn (n,p) 3.60E-06 0.72 3.68E-06 0.74 3.73E-06 0.76 3.77E-06 0.77
Mn (n,a) 9.22E-07 0.99 9.47E-07 0.98 9.59E-07 0.95 9.71E-07 0.94
Cc 6.30E-03 5.76 6.42E-03 5.86 6.48E-03 5.94 6.53E-03 6.02
(1 - Cc)-1 1.01 0.04 1.01 0.04 1.01 0.04 1.01 0.04
Mn (n,c) 1.89E-01 0.07 1.93E-01 0.07 1.95E-01 0.06 1.96E-01 0.06
1/PMn 5.30 0.07 5.18 0.07 5.13 0.06 5.09 0.06
Leakage 4.61E-02 0.58 2.35E-02 0.82 1.22E-02 1.15 6.49E-03 1.59
(1 - Ce)-1 1.00 0.03 1.02 0.02 1.01 0.01 1.01 0.01
Source absorption 1.10E-03 7.01 1.11E-03 6.92 1.19E-03 6.81 1.25E-03 6.73
(1 - Cs)-1 1.00 0.01 1.00 0.01 1.01 0.01 1.00 0.01
The symbols are defined in the text
Table 5 Result of the MCNPX calculation by using ENDF/B-VI.0 for various radiuses of manganese bath (55, 60, 65 and 70 cm) with the 252Cf
source
Reaction r = 55 cm r = 60 cm r = 65 cm r = 70 cm
Probability D (%) Probability D (%) Probability D (%) Probability D (%)
H (n,c) 7.84E-01 0.05 7.85E-01 0.04 7.86E-01 0.04 7.86E-01 0.04
O (n,c) 2.36E-04 0.05 2.36E-04 0.04 2.36E-04 0.04 2.36E-04 0.04
O (n,p) 1.89E-05 4.19 1.90E-05 4.22 1.91E-05 4.25 1.92E-05 4.27
O (n,a) 5.91E-03 0.41 5.92E-03 0.41 5.93E-03 0.41 5.93E-03 0.41
S (n,c) 7.40E-03 0.04 7.41E-03 0.04 7.42E-03 0.04 7.42E-03 0.04
S (n,p) 3.24E-04 0.23 3.25E-04 0.23 3.25E-04 0.23 3.25E-04 0.23
S (n,a) 3.10E-04 0.14 3.11E-04 0.14 3.11E-04 0.14 3.11E-04 0.14
Mn (n,p) 3.78E-06 0.55 3.79E-06 0.55 3.80E-06 0.55 3.80E-06 0.56
Mn (n,a) 9.76E-07 0.94 9.80E-07 0.93 9.83E-07 0.92 9.84E-07 0.93
Cc 6.57E-03 4.36 6.58E-03 4.38 6.59E-03 4.41 6.60E-03 4.43
(1 - Cc)-1 1.01 0.03 1.01 0.03 1.01 0.03 1.01 0.03
Mn (n,c) 1.97E-01 0.04 1.97E-01 0.04 1.97E-01 0.04 1.97E-01 0.04
1/PMn 5.08 0.04 5.07 0.04 5.07 0.04 5.07 0.04
Leakage 3.47E-03 1.53 1.93E-03 2.07 1.07E-03 2.78 6.00E-04 3.69
(1 - Ce)-1 1.00 0.01 1.00 0.004 1.00 0.003 1.00 0.002
Source absorption 1.28E-03 6.45 1.36E-03 6.38 1.43E-03 6.21 1.51E-03 6.20
(1 - Cs)-1 1.00 0.01 1.00 0.01 1.00 0.01 1.00 0.01
The symbols are defined in the text
Appraisement of the correction factors 459
123
with radiuses up to 45 cm, and for larger radiuses the fast
neutron reaction has the maximum effect.
Moreover, for the evaluation of correction factors, the
MCNPX code was used together with the neutron cross
section from other libraries, such as ENDF/B-V, ENDF/B-
VI.8 and ENDF/B-VII.0. For both types of neutron sources,
the variations of all probabilities calculated with all dif-
ferent libraries, except 16O(n,a)13C, were negligible.
The probability of 16O(n,a)13C has the main loss by the
fast neutron reactions in the bath. Therefore, the only cross
section which will introduce an appreciable error in the
correction factors is the 16O(n,a). A comparison of the16O(n,a)13C capture fraction calculated using different
libraries for the various baths with the two sources are in
Table 6. It can be observed that there is a little reduction
when using ENDF/B-VI.8 instead of ENDF/B-VI.0, and a
much greater reduction when using ENDF/B-VII.0.
Figures 2 and 3 show the probability of the total capture
reactions in oxygen and sulfur as a function of bath radius
for 241Am–Be and 252Cf source, respectively. It may be
observed that the probability of these reactions increase
with radius. Also, because of difference between energy
spectrum of two sources, for 241Am–Be the oxygen in
comparison to sulfur has a greater role in capturing the
neutron, and for 252Cf source is inverse, i.e., neutron cap-
ture of sulfur is more. This effect is because of the fission
source spectrum is fairly soft compared to the (a,n) source
spectrum and also total cross section (without elastic
scattering) of sulfur in low energy is higher than total cross
section of oxygen [5].
The probability of 1H(n,c)2d reaction as a function of
bath radius is shown in Fig. 4. As it can be seen, for 252Cf
source the rate of this reaction is more, especially for
smaller baths (This is due to 1/v form of cross section for
this reaction). The deuteron nuclei are stable and produced
gamma from it will be stopped with removing of the source
from the tank, and do not interfere in the spectrum of
gamma measured in NaI(Tl) detector. However, it should
be noted that in the long time, created deuterons will be
acted as impurities in the solution.
Figure 5 shows the probability of total capturing reac-
tions in manganese as a function of bath radius for 241Am–
Be and 252Cf source; however, the (n,c) reaction has a main
contribution of neutron capture in this nucleus. It can be
Table 6 Oxygen (n,a) capture fraction for 241Am–Be and 252Cf sources using several cross section libraries
r (cm) ENDF/B-VI.0 ENDF/B-VII.0 ENDF/B-VI.8 ENDF/B-V
241Am–Be 252Cf 241Am–Be 252Cf 241Am–Be 252Cf 241Am–Be 252Cf
35 3.87E-02 5.66E-03 2.72E-02 4.69E-03 3.41E-02 5.34E-03 2.83E-02 5.13E-03
40 3.97E-02 5.77E-03 2.75E-02 4.77E-03 3.54E-02 5.44E-03 2.96E-02 5.26E-03
45 4.02E-02 5.82E-03 2.81E-02 4.84E-03 3.63E-02 5.55E-03 2.99E-02 5.31E-03
50 4.07E-02 5.88E-03 2.85E-02 4.87E-03 3.66E-02 5.63E-03 3.01E-02 5.36E-03
55 4.09E-02 5.91E-03 2.87E-02 4.90E-03 3.68E-02 5.68E-03 3.02E-02 5.38E-03
60 4.10E-02 5.92E-03 2.87E-02 4.92E-03 3.70E-02 5.69E-03 3.03E-02 5.39E-03
65 4.11E-02 5.93E-03 2.88E-02 4.92E-03 3.70E-02 5.69E-03 3.04E-02 5.40E-03
70 4.12E-02 5.93E-03 2.88E-02 4.93E-03 3.71E-02 5.70E-03 3.05E-02 5.40E-03
Fig. 2 Total probability of interaction of neutrons with 16O and 32S
for 241Am–Be source by using ENDF/B-VI.0
Fig. 3 Total probability of interaction of neutrons with 16O and 32S
for 252Cf source by using ENDF/B-VI.0
460 R. Khabaz
123
observed that for 252Cf source, with a mean energy about
2.2 MeV, the variations of 55Mn(n,c)56Mn with radius are
less than the variations of this reaction for 241Am–Be
source, with a mean energy around 4.5 MeV [15]. So, for
calibration of radio-isotopic neutron sources with low
mean energy can be used the smaller baths. As with this
concentration of manganese sulfate, a spherical tank with
about 35 cm diameter is usable for calibration of 252Cf
source.
Figure 6 shows the probability of escape from the
boundary of bath as a function of tank radius for both
sources. For both types of neutron sources, the statistical
uncertainty of the leakage probabilities calculated with four
different libraries, i.e., ENDF/B-VI.0, ENDF/B-V, ENDF/
B-VI.8 and ENDF/B-VII.0, was 0.18 % or less.
As it can be seen, the leakage of neutron is decreased
with radius. If the leakage from the bath must be less than
about 1 % [16, 17], then for having a suitable efficiency in
calibration of 241Am–Be source (according to Fig. 5 the
slope of radius larger than 60 cm is negligible), the radius
of tank with this concentration can be about 60–65 cm.
During this work, it was observed that the probability of
leakage (Ce) could be well fitted as a function of sphere
radius by the following exponential equation
Ce ¼ Co: exp � r � ro
t
� �ð5Þ
where r is the bath radius (cm) and Co, ro and t are
parameters that for two sources, based on results calculated
with ENDF/B-VI.0, are listed in Table 7.
Conclusions
The correction factors of some manganese bath system for
various radiuses have been calculated using a recent cross
section library by Monte Carlo MCNPX code. In the
simulations it was assumed that 241Am–Be and 252Cf
sources with different energy spectrum (mean energy of
about 4.5 and 2.2 MeV) have been located in the center of
manganese tank. Various objects affecting the manganese
activity of the bath have been calculated and studied, such
as (n,c), (n,p) and (n,a) reaction in the nuclei of the com-
ponents of the solution, neutron recaptured by the source
and its mounting assembly, and neutron leakage from the
boundaries of the bath. Although the calculation has been
Fig. 4 The probability of 1H(n,c)2d reaction as a function of bath
radius for two sources by using ENDF/B-VI.0
Fig. 5 The probability of 55Mn(n,c)56Mn reaction as a function of
bath radius for two sources using ENDF/B-VI.0
Fig. 6 The probability of leakage from the bath as a function of tank
radius for two sources calculated with different libraries
Table 7 Fitting parameters of Eq. (5) for the calculated leakage Ce
versus bath radius r with ENDF/B-VI.0
Source Co ro t
241Am–Be 0.1526 ± 0.0003 35.0 10.12 ± 0.04252Cf 0.0460 ± 0.0002 35.0 7.59 ± 0.06
Appraisement of the correction factors 461
123
performed only for one concentration of MnSO4 in the
solution [93.68 g/(kg of Solution)], the simulation can be
generalized for other concentrations. Maximum probability
of neutron capture was for hydrogen nuclei that the result is
the production of deuteron impurity; therefore, the ratio of
NH/NMn in manganese solution is the one of important
parameters.
The difference of the probability of all events, except16O(n,a), calculated by considering of various libraries was
insignificant; however, determination of the 16O(n,a)13C
reaction probability is one of the important challenges in
the manganese bath. It was observed that there is a slight
reduction when using ENDF/B-VI.8 instead of ENDF/B-
VI.0, and a much greater reduction when using ENDF/B-
VII.0; however, the results calculated using ENDF/B-V
and ENDF/B-VII.0 were approximately agreement. For252Cf source in compared to 241Am–Be, the differences
were less.
Also, the calculations described in this report have
shown that with this concentration, for calibration of 252Cf
and 241Am–Be source the spherical bath by 35 and
60–65 cm radius is proper, respectively.
References
1. Khabaz R, Miri H (2011) Development of a Bonner sphere
spectrometer with emphasis on decreasing the contribution of
scattering by using a new designed shadow cone. J Radioanal
Nucl Chem 289:789–794
2. Khabaz R, Miri H (2011) Measurement of neutron spectrum with
multi-sphere using BF3 and evaluation of scattering effect on
spectrum. Nucl Technol Radiat Prot 26:140–146
3. Axton EJ, Cross P, Robertson JC (1965) Calibration of the NPL
standard Ra–Be photoneutron source by an improved manganese
sulfate bath technique. J Nucl Energy 19:409–422
4. Firestone RB (1996) Table of isotopes, 8th edn. Wiley-Inter-
Science, New York
5. Experimental Nuclear Reaction Data (EXFOR), Database Ver-
sion of April 05, 2010
6. Kil-Oung C, Young-Seok L, Sun-Tae H, Kwang-Pil L, Keung-
Shik P (1999) Impurity correction factor of MnSO4 compound for
the determination of neutron emission rate on the manganese bath
method. J Radioanal Nucl Chem 239:605–608
7. Tae SP, Jong ML, Han YH (2002) Standardization of 152Eu and88Y. Appl Radiat Isot 56:275–280
8. Axton EJ, Bardell AG, Felgate SJ, Long EMR (1985) The ratio of
the thermal neutron capture cross-sections for hydrogen and
manganese and its impact on the measurement of neutron source
emission rates by manganese bath techniques. Metrologia
21:181–191
9. De VA, Porges KG (1969) Absolute calibration of neutron
sources having a wide range of emission spectra. Metrologia
5:128–141
10. Waters LS (2002) MCNPX-A general Monte-Carlo N-particle
transport code, Version 2.4.0, LANL report LA-CP-02-408, Los
Alamos
11. ISO 8529-2 (2000) Reference neutron radiations-part 2: calibra-
tion fundamentals of radiation protection devices related to the
basic quantities characterizing the radiation field. International
Organization for Standardization, Geneva
12. Robert NJ (2001) MCNP calculations of corrections factors for
radionuclide neutron source emission rate measurements using
the manganese bath. NPL Report CIRM 45, Teddington
13. McGarray ED, Boswell EW (1988) NBS measurement service:
neutron source strength calibration. NBS Spec Publ 250:18
14. Sun-Tae H, Kun JaiL (1988) Absolute neutron emission rate
measurement of a 252Cf source by the manganese sulfate bath
method. Nucl Instr Meth Phys Res A 273:381–388
15. International Atomic Energy Agency (IAEA) (1970) Neutron
moisture gauges. Technical Report Series No. 112, Vienna
16. O’neal RD, Scharff-Goldhaber G (1946) Determination of
absolute neutron intensities. Phys Rev 69:368
17. Park H, Choi K-O, Lee J-M, Lee KB, Hahn MS (2005) Absolute
measurement of the neutron emission rate with a manganese
sulfate bath system. J Korean Phys Soc 47:603–609
462 R. Khabaz
123