CHINESE JOURNAL OF PHYSICS

VOL. 11, NO. z

OCTOBER 1973

Absolute Determination of the Fast Neutron Fluxes by Using the Flow-Type Manganese Bath Method
M I E N- WIN WV ($%%:a) and JE N- CHANG CHOU (fiG+)
I&it&e of Nuclear Energy Research, Atomic Energy Council P. 0. Box 3 Lung-Tan, Taiwan

(Received 12 August 1973)

The absolute neutron flux produced in a Van de Graaff accelerator via the Li (p, n) B e-reaction was measured with the help of a circulated manganese bath. An elaborate process was developed for the absolute determination of the efficiency of the gamma detector adapting the circulating system. The absolute emission rate of an Am-Be neutron source was also determined with the bath method, which agrees well with the calculated value according to the given decay rate of 2rlAm.

I. INTRODUCTION

the determination of the absolute neutron fluxes, three principal methods IFOR are available. These are: 1) the associated particle method, 2) the standard cross section method, and 3) the bath method. The great advantage of the bath method is its flat response throughout the entire energy range from thermal up to several .million electron volts. Due to the large and accurate thermal neutron cross section of manganese, the manganese bath method is particularly useful in fast neutron range from 1 keV to 10 MeV. A circulation system was built, which enables us to measure the induced activity of manganese continuously during irradiation. An elaborate process was developed for the absolute determination of the efficiency of the gamma detector adapting the circulating system. In this experiment, two groups of neutron fluxes with neutron energies of 1X&40 keV and 807k40 keV were determined by the bath method. The emission rate of an Am-Be neutron source was also measured with the same solution of manganese sulphate. The result agrees well with the calculated value.
II. THEORY

The principle of the manganese bath method is that the incident neutrons, after entering the bath, are thermalized and captured in an aqueous solution of manganese sulphate by various nuclei present in it. A certain fraction of that is captured by 55Mn. The absolute disintegration rate of the resulting 56Mn gives the information of the total incident neutron flux. 97

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THE FLOW-TYPE MANGANESE BATH METHOD

The neutron capture rates of various nuclei present in the solution were determined by the relative concentrations and their thermal neutron capture cross sections. The fraction of neutrons that is captured by manganese is given by the relation
f=

N MnuYn(l+al
Nm,[ua(l+a) +os+4uol+N H

uH+A-uo +Nm um+~us+zuo 2 ) 2 ) (

(1)
,

where NH,,, NH, and N,, are, respectively, the number of nuclei of manganese, hydrogen, and sodium per milliliter in the solution and uy,, US, OH, u. and UNa are the thermal neutron capture cross sections of manganese, sulphur, hydrogen, oxygen and sodium, respectively. The factor (l+a) is a non-l/v correction factor, which was taken from Ref. (1). Let C(T1, Tz, Td be the total counts of the gamma detector from time TI to Tz, under irradiation-time T3. After correction for the effects of background, dead time, and Compton signal of sodium, then the average neutron flux dav at the bath entrance, which corresponds to an average monitor counting rate, is given by @= EM,

Sf

C (Tl, Tz, Ts) (1 - L) A CT,, Tz, Td ,

(2)

where cy, is the efficiency of the gamma detector for 0.845 MeV gamma. S is the area at the surface of the bath from which neutrons can enter into the bath. f is the fraction df neutrons that is captured by manganese as given by Eq. (1). L is the fraction of neutrons that leaks from the boundary of the bath. A(TI, Tz, T3) is a time-dependent factor which is given by

prp +

(l-e-At )dt

with
/l=R+-

vbr,

vc .

In these equations, i. is the decay constant of 56Mn. vb is the volume of the

( 1 ) E. J. Axton, P. Cross and J. C. Robertson, J. of Kucl. Energy, Parts A/B 19 409 (1965).

M. W. WU AND J. C. CHOU

99

the bath, Vd is the volume of the container surrounding the gamma detector. Jc is the sum of Vd and the volume of the all pipes of the circulation system. Vi is the total volume of the circulation system. T is the sampling time-interval. TI=mT is the time of the beginning of the counting. Tz is the time of the ending of the counting. T3=nT is the time of the ending of the activation. Ci is the average counting rate in monitor at i-th time-interval. C,, is the average counting rate in monitor over all the time of irradiation. rp is the time required for solution to be pumped from the bath, through the counter, and back to the bath. Between T and rp there exists the relation T = (k + P) rp where k is the integral part, and P is the decimal part. In the derivation we assumed tacitly that once a neutron entering the bath, it will either be captured or leaked from the surface of the bath. Since the incident neutrons have an energy below the effective threshold for (n, P) and (n, a) reactions in manganese, sulphur, oxygen and sodium. It is also found that the leakage of neutron from the spherical bath of 60 cm diameter is less than 1 10. O The effect of different incident neutron energies needs not to be considered in calculating the neutron fluxes. This is a very desired characteristic of this method, and thus the errors introduced by the uncertainty of the fast neutron capture cross section could be greatly reduced. III. EXPERIMENTAL METHOD 3-l Apparatus and experimental procedure The circulation system contains a large hollow aluminum sphere of 60 cm in diameter, where the aqueous solution of manganese sulphate is activated, and a small aluminum container, where the activity of 56Mn is measured. These two containers were connected by a 2.1 cm dia. PVC pipe of 50 meter long. The volumes of the spherical bath and the cylindrical container are 101.5 liters and 9.74 liters, respectively. Their inner sides are coated with epoxy-resin to prevent corrosion. A cone-formed vacancy is left, which extends from the surface into the center of the bath, to let the neutrons enter directly into the bath (See Fig. 1). The neutron leakage from this cone is less than 0.1%. A cylindrical collimator of 50 cm in length and 60 cm in diameter was used between the neutron source and the bath. The composition of the collimator is a mixture of 50% paraffin and 50% LiCOa in weight. A paraffin plug was also prepared for the measurement of neutron background. (4)

100

THE FLOW-TYPE MANGANESE BATH hlETHOD

'solution in

101.5 liters metal-Li

proton beam

4luminnm spherical bath collimator made of a mixture 0.f paraffin and lithium carbonate I I c

t-50 cn++---50 cm -

\ 0.5 mm Zd-absorber

yrr
Sol i o n out

Fig. 1. Experimental arrangement for the activation of the solution of manganese surphate in bath method

The setup of the circulation system is shown in Fig. 2. The solution was pumped by a *HP water-pump in a closed circuit through a 4 x 3 NaI(T1) detector. The flow rate of the solution was estimated to be 40 liters per minute. The time required for the solution to flow from the bath to detector is less than 21 sec., thus the decay of the activity of 56Mn (T.;- =2.57hr.j in transferring from bath to detector may be neglected. The signal of the 0.845 MeV gamma ray following the decay of 56Mn is led to a preamplifier and a linear amplifier, and then is fed to a multichannel analyzer_ The area under the 0.845 MeV is a measure of the activity of 5Mn. 3-2 Determination of the efficiency of the gamma detector The efficiency of the gamma detector for the circulated manganese sulphete after activation, Ed,, was determined directly by putting a known amount of uniformly distributed 56Mn nuclides into the container. The same geometry in detection provides a direct interpretation of the efficiency. After irradiating 55Mn in a thermal reactor, the amount of Mn was determined in a 4xP-r coincidence

paraffin or about 25 cm in thickness

concrete wall o f a b o u t 30 cn i n thickness

50 cm (paraffin + Li2C03) -shielding

4 x 3 i n . Nal

25 meter

5 cm Pb-shielding Fig. 2. The circulation system of manganese bath

unit. In order to minimize the B- self absorption, a thin foil of manganese was prepared by using the vacuum evaporation technique. The backing is an aluminum foil of 190 yg/cm in thickness. The purity of the manganese metal for evaporation was assayed to be no less than 99 K. The thickness of the layer of manganese on aluminum backing was measured to be about 200 pug/cm. Thus the total thickness of the prepared foil is about 400 pg/cm, which is suitable for 8-r coincidence measurement. The foil of known activity was then dissolved in 40 ml of HzS04. The concentration of HzSOa is about 8N. After dissolving completely, it was diluted to 9.74 liters with distilled water. The solution was poured into the cylindrical container, where the gamma activity of the circulating fluid was measured. After correction for the decay of the 56Mn, the &ciency of the gamma detector can be obtained directly. 3-3 The analysis of the concentration of the aqueous solution of manganese sulphate By the method of the atomic emission spectrum, the concentration of the solution was semi-quantitatively determined. For the accurate determination of the concentrations of manganese and sodium, the neutron activation analysis in

102

THE FLOW-TYPE MANGANESE BATH METHOD

a thermal reactor was used. Thus its relative disintegration rates in comparison with those of standard solutions, with were obtained by using a Ge(Li)-detector, yield the accurate values of the concentration of Mn and Na in the aqueous solution. IV. RESULTS The best set of data used for the determination of the over-all efficiency of x 3 NaI(T1) -detector of 0.845 MeV following the decay of 56Mn are listed in 4 Table 1. Here Ni, N; and NZ are the background-corrected counting rate in P, r and coincidence channel, respectively. The loss in counting rate in P and coincidence channels as well as the counting rate of the chance coincidence are also included. After these corrections, NB, N,, and N, give the true counting rate in each channel and the absolute disintegration rate of the sample, No, at that time is obtained. It also shows the absolute disintegration rate of the sample, R, at the reference time when the counting rate of the sample is measured in the 4 x 3 NaI(T1) detector and thus the efficiency is calculated. The error of cy, is estimated to be 1.7%.
Table 1.

Counting rate with 477 /3-r detectors and the efficiency calculated
(all counting rates are in counts/set) Nj = (1.47 * 0.02) x 10 Nr = (1.852 z!z 0.006) x 10 Nc = (1.64 i 0.003) x 10 No = (1.66 f 0.03) x 10

N; = (1.313 & 0.006) x 10 N; = (1.852 & O.bG6) x 1C2 Iv; = (1.543 f 0.005) x 102 loss of counting rate in B-channel = (1.540 & 0.003) x 10~ 10~s of counting rate in coincidence channel = (1.95 & 0.64) x 10 counting rate of chance coincidence = 9.73 & 0.97

R = (5.65 z!z 0.10) x lo*

c o u n t i n g r a t e i n 4 x 3 NaI(T1) detector = (4.667 III 0.012) X 10 EM,, = (8.25 Z!I 0.14) x 10-a

By activation analysis, the concentration of manganese is (2.32kO.18) x 1 0 mg/ml, and that of sodium is (5.21i0.16) x 10 mg/ml. For the calculation of the fraction of neutrons absorbed by manganese, the published values for the thermal neutron capture cross rection are adopted. They are uMn = 13.2 L 0.4 barn() = 0.49 barnc4) (JS = 0.000178 barnc5) 00
OH

0.332 barnc3) uKa = 0.56 barnc5)

=

The non-l/v correction factor (l+d) is found to be 1.0106 at this concentration of the solution (1). The calculated value of f is 0.134i.O.003.
( 2) (3 ) ( 4 ) (5) J. D. D. S. D. Juren and J. Chin, J. Res. Natl. Bur. Stand. 55, 311 (1955). J. Hughes and R. B. Schwartz S upplement No. l, BNL 325 (1957). J. Hughes and J. A. Harvey, BNL 325 (1955). Glasstone and A. Sesonske NucIear Reactor Engineering (1962).

M. W. WU AND J. C. CHOU

103

The neutron leakage measured is less than one percent, hence it is neglected in the calculation. The data needed for the calculation of the neutron fluxes as well as the resulted average neutron fluxes at each bombarding energies of protons are given in Table 2 and Table 3. Table 2. The data needed for the calculation of neutron flux and the resulted
neutron flux at Ep=1.97 MeV
Neutron background -. Counting rate in monitor T1 TZ Ts (7.78 h 0.05) x lOr/sec. 10620 sec. 2 2 7 2 0 1 4 6 0 0 s e c . s e c .

(a)

neutron background and neutrons through collimator ._ _~ (7.37 * 0.05) x lOl/sec. 10530 sec. 16560 sec. 14670 sec. (5.50 Zb 0.02) x 10 (3.25 i 0.02) x lo* (1.69 & 0.01) x 10 (1.69 & 0.01) x 10

tb)

Net

neutrons

(7.37 i 0.05) x lOi/sec.

Tz, Ta) ACT,, Tz, Ts)

C,T,, C/.4 before normalization C/A after normalization

(2.89 f 0.02) x 10 (5.25 & 0.03) x lo2 (5.50 i 0.03) x 10 (5.21 + 0.03) x 10

; )
~

(1.17 zt 0.007) x 10 (2.75 & 0.17) X 1Oa (c)

%p-) set-cm2

/ (a) It is measured with paraffin plug in the collimator. (b) It is measured with collimator open. (c) It is the neutron flux at 1 meter from the target when average proton current is 2 target thickness is 40 keV at threshold energy. Table 3.

pA a n d

The data needed for the calculation of neutron flux and the resulted neutron flux at Ep=2.52 MeV ,(b) Neutron background I (a) Net neutrons
Neutron background and neutrons through collimator (1.93 * 0.01) x 10Z/sec. 6850 sec. 21970 17480 sec. (4.67 f- 0 02) x 10 (8.01 + 0.04) x l@ sec.

Counting rate in monitor T1 T? T, C(T,, Tz, 2s) AiT,, Tt, Tz) C/A before normalization

/ (2.00 * 0.01) x iO*/sec. I I i : / ~

5700 sec. 14760 sec. 14590 sec. (8.28 & 0.03) x lo (4.46 f 0.02) x lo2

(2.00 & 0.01) x lO?/sec.

(1.85 & 0.01) x 10Z (5.83 i 0.03) x 10 C/A after normalization / (1.85 & 0.01) x 10 (6.04 i C.04) x 10 , 72 mu* ( ~ set-cm* > 1 * The specifications of (a), (b) and (c) are the same as in Table 2.

(1.25 + 0.007) x 10 (2.94 Zh 0.18) x 10 (c)

According to the data given in Ref. (6), the neutron leakage of the Am-Be neutron source in the given bath is estimated to be 11%. The fast neutron loss due to (n, p) and (n, a) reactions in sulphur and oxygen is found to be about
( tj ) A. De Volpi, Proc. of the EANDC Conf. on Xeeutron Stand. and Flux Normalization, Argonne U. S. A. (Aug. 1971) p. 470.

AL--

104
3.3 o/6 in Ref.

THE FLOW-TYPE MANGANESE BATH METHOD

(7). The measured emission rate of the Am-Be neutron source is Q = (1.02 -t 0.03) x lo6 neutrons/set.
V. DISCUSSJON AND ERROR ESTIMATION

It is found in Ref. (8) that the maximum neutron yield obtained from an Am-Be source is about 74 neutrons per lo6 alphas. The radioactivity of the given source is 400 mc. It follows that its maximum neutron emission rate is 1.09x lo6 neutrons/set. The measured emission rate of (1.02 * 0.03) x lo6 neutrons/set. agrees well with the predicted value.
Other sources of error are: 1. The high flow rate of the circulation system causes the solution not to

be mixed homogeneously before it flows out of the bath, and thus reduces the effective volume of activation. 2. There is a certain amount of neutrons scattered from the inner surface of the collimator. These scattered neutrons may enter into the bath and cause activation. Both effects will result a higher measured neutron flux than the actual one. The former effect is estimated to be less than 4 % which is proved by the measured emission rate of Am-Be neutron source. The later effect is calculated to be less than 0.5%. Summing up all kinds of possible errors, an accuracy of less than 6% can be obtained in the determination of the absolute fast neutron flux.
ACKNOWLEDGEMENTS

The authors wish to thank Dr. J. P. Chien, director of the Institute of Nuclear Energy Research for his support of this work. To Accelerator Group and ZPR reactor group in the same Institute, we wish to express our sincere thanks for their assistance during the course of experiment. Special appreciations are extended to Mrs. Shirley L. Lee and Mr. Sung-Yin Tang for their careful analysis of the solution of manganese sulphate by emission method.

(7 j K. W. Geiger and A. I. Baerg, Can. J. Phys. 43. 375 (19Gji. (8) 0. J. C. Runnalls and R. R. Boucher, Can. J. Phys. 34, 949 (1956).