Continental J.

Applied Sciences 6 (2): 60 - 65, 2011 Wilolud Journals, 2011 Printed in Nigeria

ISSN: 1597 9928 http://www.wiloludjournal.com

EFFECT OF NUCLEAR DATA ON CALCULATED K0-VALUES A. Avaa, U. Sadiq, and T.S. Azande Department of Physics, Ahmadu Bello University, Zaria, Nigeria

ABSTRACT In order to validate the use of experimental k0-values for INAA instead of calculated k0-values using nuclear constant from literature, the k0-values for these nuclides 49Ca , 131Ba , 115C, 152Sm , 75Se , 116mIn, 134 Cs suspected to be discrepant were measured using Synthetic multi-elemental Standard (SMELS) and Standard reference material, Coal Fly ash (1633b). Result obtained compare more favourably with the recently recommended values than the calculated values, thus confirming the fact that some of the nuclear constants have to be remeasured KEYWORDS: k0-values, nuclear data, discrepant nuclides, SMELS, Standard reference material INTRODUCTION In Neutron Activation Analysis (NAA), concentration of elements in samples was determined using short, medium and long lived activation products. The concentration of elements is mainly determined by Absolute, relative or single comparator and k0-NAA method (De Corte and Simonits, 2003). In the absolute method, the concentration of elements in a sample can be calculated with the activation and decay equation provided the reaction rates, detector efficiency curve, half-lives, and decay schemes of radionuclide are known (Acharaya et al, 2010). The reaction rate can be determined by measuring the neutron fluxes with monitor elements like Au, which is co- irradiated with samples. If the nuclear parameters are precisely known, then this method can yield accurate concentrations for elements in the sample. In practice, however, uncertainties in the nuclear parameters can easily affect the accuracy for determining the concentration of an element of interest (IAEA, 1990). In the relative or comparator method, samples are irradiated simultaneously with standards containing known amounts of elements. After irradiation, both samples and standard are measured under identical geometrical conditions with the same detector. This procedure eliminates uncertainties in the nuclear parameters, detector efficiencies, etc. This method is still being regarded as one of the methods which have the highest accuracy of NAA (Dung and Hien, 2003). However, the method still has some setbacks, because it requires a large number of individual element standards or use of a well-characterized multi-element standard (IAEA, 1990). Preparation and irradiation of individual standards for each element are time consuming and expensive; and the use of reference materials is not always practical because of the limited accuracy for certain elements or the difference between sample and standard matrices. As a result the k0 NAA method was developed. This k0-NAA method is based on co-irradiation of the sample and a neutron fluence rate monitor and on using an experimentally determined composite nuclear constant [k0.n(a)] (Moens et al, 1983) the establishment of this method holds the following merits: i. The troublesome preparation of chemical standards can be avoided. ii. The radioactivity counting time for standards can be saved. iii. Quantitative results for elements, but absent in chemical standards can be obtained. iv. Some nuclear parameters, e.g. the cross-section of neutron capture reaction and the branching ratio of the gamma-ray emitted by the radioactive nuclide, can be re-evaluated. In this work, the k0-values of some nuclides were calculated using published nuclear data in (IAEA, 1974; Glascock, 1996 and Blaauw, 1996) and measured using Synthetic Multi - element Standards (SMELS), which is the reference materials recommended by the International k0-user Community for the validation of k0 NAA method

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A. Avaa et al.,: Continental J. Applied Sciences 6 (2): 60 - 65, 2011

and the standard reference materials , NIST-1633b (Coal Fly Ash) with NIRR-1 facilities.NIRR-1 is the commercial version of the Chinese made Miniature Neutron Source Reactor (MNSR). It is moderated and cooled by light-water and reflected by beryllium. Theoretical consideration The k0-factor can be determined by calculation using

k0 =

M Au * * * th M * Au * Au th ( Au )

Where, th = thermal absorption cross section for neutron (velocity 2200m/s),

atomic weight and = gamma-ray intensity. These parameters are taken from literature. The k0-values can also be determined using the Hogdahl formalism.

= isotopic abundance, M =

k0.Au =

(N P

(N

Wt m SDC ) Au f + Q0.a ( ) Au Au

Wt m SDC )a f + Q0. Au ( )

Where, W = mass of the element, Np = net number of counts in the full energy peak, p = full energy peak detection efficiency, S = 1= Saturation factor, tirr is the irradiation time, D = = decay factor with td decay time, C = = counting time correction, tc is the counting time, = thermal to epithermal flux ratio, Q0() = the ratio of resonance integral to thermal cross-section corrected for non-ideal epithermal neutron flux where is epithermal neutron shape factor which is calculated (Jonah et al, 2005 and Moens et al, 1983) using Q0() =

Q0 0.429 Er

Where, E r is the effective resonance energy. The net peak area (Np) corresponding to the photo peak which is calculated by summing the counts under the peak and subtracting the linear Compton background was used to calculate the specific count rate (Asp) shown in the expression below: Asp = 4

The result of this work was compared with the recommended data using the student t-test , the expression for the t-test is shown below:

t=

d Sd n

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A. Avaa et al.,: Continental J. Applied Sciences 6 (2): 60 - 65, 2011

Where

= average difference given as:

d
n

2 d

(d =

d N 1
i

The hypothesis for the t-test is stated as follows: H0: all di = 0; there is no difference between the calculated, measured k0-value and the recommended values. H1 : all di 0; there is a significant difference between the calculated, measured and the recommended values. This is a null and alternative hypothesis, this means for the null hypothesis, when t-cal.> tcritical reject H0 and for the alternative hypothesis, when t-cal.< tcritical, accept H0. METHODOLOGY Known amount of gold, SMELS type III and Coal fly ash equivalent to 200mg was wrapped in polyethylene films, which have been cleaned appropriately. Two samples each were prepared for long and short irradiations. Irradiation of samples was done using Nigeria Research Reactor-1 (NIRR-1) operating at half-full power of about 15kw with neutron flux 5 1011n/cm2.s. Two regimes of irradiation depending on the half - life of product radionuclide were adopted. The short irradiation was performed in the outer irradiation channel B4, where the population of fast neutron flux is small thereby minimizing interference caused by threshold reactions with an irradiation time of 1 minute. For elements that produce long-lived nuclides, the irradiation is performed for 6 hours in the inner irradiation channel B2, where the magnitude of the thermal neutron flux is highest. After irradiation, induced activities in detector foils were measured on a GEM-30195 HPGe Coaxial, vertical dipstick detector (Ortec), which has a relative efficiency of 30% and resolution of 1.95Kev at 1-33Mev, 60Co. The gamma-ray acquisition system consists of the MAESTRO emulation software compatible with Multi-channel Analyzer (MCA) and a personal computer was used for peak identification and evaluation. Two gamma-ray measuring procedures were employed for the counting of short-lived nuclides. The first procedure, S1 was performed at sample-detector geometry of 5cm for 10minutes, after a delay time of 2-15 minutes. The second procedure, S2 was performed also for 10minutes but a sample detector distance of 2cm following a waiting time of 3hours, 35minutes. For the long-lived nuclides, the gamma-ray measurements are performed at sample-detector geometry of 1cm for 30minutes after a waiting period of 5-6 days, which has been designated as protocol, L1. The second protocol, L2 gamma-ray measurement is performed at the same geometry for 1 hour, after a delay time of 910 days. RESULTS AND DISCUSSION The relevant data used for the calculation of k0-values are given in Table 1. In Table 2 the calculated k0-values using equation [1] were compared with the recommended values. Significant deviations ranging from -10.2% -98.7% were observed. This large deviation demonstrates the unreliability of randomly chosen nuclear data as reported in Moens et al, 1983. Table.3 present measured k0-values from Coal Fly Ash and SMELS, the Q0-values used were taken from literature (De Corte and Simonits, 2003) and corrected for non-ideality of epithermal neutron flux. Specific activities were computed by substituting the measured peak area into equation [4]. The k0-values were calculated by imputing the specific activities into equation [1] using MICROSOFT-EXCEL. In Table 3, column 4 shows the measured k0 values from SMELS and Coal Fly Ash with their uncertainties. The major source of uncertainty in this work is that due to peak area analysis and from a determination of overall, and values used. The results compare well with the recommended data for most nuclides. A two-tailed student t- test was the statistical analysis used to test for the level of significance; a confidence interval of 5% was chosen, which represent t0.025. From the t-table (abridged from Table 3 of Fisher and Yates), for 5% level of significance and 14

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A. Avaa et al.,: Continental J. Applied Sciences 6 (2): 60 - 65, 2011

degree of freedom (df), tcritical is given as: t0.025,14 = 2.145, this value is greater than the calculated t-value of 0.038339 from the experimental values, it was concluded that the result was not significant at 5% level. That is to say, the null hypothesis is accepted. From the calculated k0- values, t-value was found to be -0.00467, this value. is less than tcritical above, this shows a significant difference between the calculated and recommended k0-values, thus the alternate hypothesis is accepted. Table 1: Nuclear data used for the calculation of k0-values Formed T1/2 E(keV) Ma Target a a a Nuclide isotope

Q0

Se-74

Se-75

119.8d

121 136 265 279 401

78.96 78.96 78.96 78.96 78.96

17.2 59.0 59.1 25.2 11.5

9.00E-3 9.00E-3 9.00E-3 9.00E-3 9.00E-3

5.04E+1 5.04E+1 5.04E+1 5.04E+1 5.04E+1

11.5 11.5 11.5 11.5 11.5

Ba-132

Ba-131

11.5d

124 134 216 373 486 496 620 417 1097 1293 563 569 605 796 802 103 3084

137.33 137.33 137.33 137.33 137.33 137.33 137.33 114.82 114.82 114.82 132.9054 132.9054 132.9054 132.9054 132.9054 150.36 40.0780

29.1 2.2 19.9 13.3 1.9 43.7 1.6 30.0 56.2 85.1 8.4 15.4 97.5 85.3 8.7 37.0 92.1

1.06E-3 1.06E-3 1.06E-3 1.06E-3 1.06E-3 1.06E-3 1.06E-3 9.57E-1 9.57E-1 9.57E-1 1.00E-1 1.00E-1 1.00E-1 1.00E-1 1.00E-1 2.67E-1 1.87E-3

7.54E+00 7.54E+00 7.54E+00 7.54E+00 7.54E+00 7.54E+00 7.54E+00 1.54E+2 1.54E+2 1.54E+2 3.04E+1 3.04E+1 3.04E+1 3.04E+1 3.04E+1 2.20E+2 1.12E+00

21.3 21.3 21.3 21.3 21.3 21.3 21.3 16.8 16.8 16.8 12.7 12.7 12.7 12.7 12.7 14.4 0.5

In-115

In-116m 54.15m

Cs-133

Cs-134

2.062y

Sm-152 Sm-153 46.5h Ca-48 Ca-49 8.71m

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Table 2: Comparison of the calculated k0-values with recommended values Target T1/2 E(keV) Cal. K0-values Recom. % dev Nuclide Values Se-74 119.8d 121 136 265 279 401 124 134 216 373 486 496 417 1097 1293 563 569 605 796 802 3084 2.61E-3 8.96E-3 8.97E-3 3.83E-3 1.75E-3 4.48E-5 3.35E-6 3.06E-5 2.05E-5 2.89E-6 6.72E-5 1.02E+00 1.91E+00 2.89E+00 5.07E-2 9.31E-2 5.89E-1 5.16E-1 5.28E-2 1.27E-4 1.94E-3 6.76E-3 7.11E-3 3.00E-3 1.43E-3 3.90E-5 3.24E-6 2.75E-5 1.92E-5 3.44E-6 6.48E-5 7.54E-1 1.60E+0 2.29E+0 4.14E-2 7.34E-2 4.76E-1 4.15E-1 4.11E-2 1.01E-4 -34.6 -32.5 -26.2 -27.6 -22.1 -14.8 -35.0 -11.3 -65.6 15.9 -37.4 98.7 -19.2 -26.1 -22.5 -26.9 -23.8 -24.3 -28.4 -26.0

Ba-132

11.5d

In-115

54.15m

Cs-133

2.062y

Ca-48

8.71m

Table 3: Comparison of experimental values and calculated k0-values with recommended values Recom. k0-values (De Corte and cal. k0formed Energy values Simonits; 2003) Expt. k0-values Isotope (kev) Se-75 121 136 401.73 373 486 496 417 1097 1293 562 569 602 802 (1.94E-3) (6.76E-31.1) (1.43E-10.8) (1.92E-50.4) (3.44E-6) (6.48E-50.2) (7.54E-11.1) (1.60E+01.3) (2.29E+00.8) (4.14E-21.7) (7.34E-21.5) (4.67E-12) (4.11E-22) (1.01E-40.9) BDL (6.88E-31.1) (1.38E-30.7) (1.95E-50.6) (3.43E-60.2) (6.45E-50.2) (7.27E-10.9) (1.54E+01.2) (2.28E+000.7) (4.00E-21.4) (7.32E-21.5) (4.67E-11.8) (3.93E-21.8) (1.10E-41.4) 2.61E-3 8.96E-3 1.75E-3 2.05E-5 2.89E-6 6.72E-5 1.02E+0 1.91E+0 2.89E+0 5.07E-2 9.31E-2 5.89E-1 5.28E-2 1.27E-4

Ba131

In-116m

Cs-134

Ca-49 3084 BDL: Below Detection limit

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A. Avaa et al.,: Continental J. Applied Sciences 6 (2): 60 - 65, 2011

CONCLUSION The k0-values of some nuclides were calculated and re-measured using Certified Reference Materials, (SMELS III and NIST 1633b Coal fly Ash), results obtained from the statistical analysis using student t- test at 5% confidence interval affirms the null hypothesis. Meaning there is no significance difference with the re-measured k0 values and the recommended data. On the other hand, the alternate hypothesis was accepted when the calculated k0-values were compared with recommended values at the same confidence interval, this means there is a significant difference between the calculated and recommended values. This shows how unreliable some of the nuclear data used for the calculation of k0-values are. We recommend that some of nuclear data need to be remeasured by International k0user Community. REFERENCES Acharya, R., Swain, K.K., Amit, K., Nicy, A., Verma, R., Reddy, A.V.R. (2010). Journal of Radioanal.Nucl. Chem. DOI 10.1007/S10967-010-0790-3 Blaauw, M., (1996). The k0-consistent IRI gamma-ray catalogue for INAA; CIP-DATA KONINKLIJKE BIBLIOTHEEK, DEN HAAG, Netherland. De Corte, F., Simonits A. (2003). Recommendd data for use in the k0-standardization of neutron activation analysis, Atomic Data and Nuclear Data Tables 85: 47 67 www.sciencedirect.com Fisher & Yates : Statistical Tables for Biological, Agricultural and Medical Glascock, M.D., (1996). Tables for Neutron Activation Analysis. The University of Missouri Research Center: Columbia, MO.S Ho Manh Dung, Pham Duy Hien; (2003). Journal of Radioanalytical and Nuclear Chemistry 257: 643-647 IAEA Handbook of Nuclear Activation Cross Section (1974) 156. IAEA, (1990). Technical corporation activities. Jonah, S.A. Balogun, G.I., Umar, I.M. Mayaki, M.C. (2005). Journal of Radioanal. And Nucl Chem.266:83-8 Moens, I., De Corte, F., De Wispelaere, A., Hoste, J. (1983) in k0 Measurements and related nuclear Data Compilation for (n,) Reactor Neutron Activation Analysis Part II, National Fonds voor Wetenchappelijk Onderzoek: 386-411. Research. Oliver & Boyd Ltd. Edmburgh. Simonits, A., De Corte, F., Hoste, J. (1975). Single Comparator methods in Reactor Neutron Activation Analysis. Journal of Radioanalytical Chemistry 24:31 46. Received for Publication: 26/04/11 Accepted for Publication: 16/06/11 Corresponding Author A. Avaa, Department of Physics, Ahmadu Bello University, Zaria, Nigeria Email: avaab2003@yahoo.com

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