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Phương pháp trùng hợp cc (phát hiện hai ctia phát ra gần như đồng thời) đã được sử dụngtrong nghiên cứu cấu trúc hạt nhân 1, và cũng là một điểmsible cách để cải thiện độ nhạy cảm của dấu nhắckỹ thuật phân tích kích hoạt gamma (PGAA) 2.Là một phần của cơ sở cho các neutron gây raquang phổ tia gamma (NIPS) tạiCổng chùm PGAA của Budapest Reac nghiên cứutor một cc coincidence bộ máy đã được phát triển.Trong các bài viết trước của chúng tôi, đồng xu cc khu vựcphương pháp cidence được giới thiệu 2, và meathiết lập bảo đảm đã được mô tả chi tiết 3. Trongbài báo hiện tại chúng tôi trình bày một phép đo clo để minh họa chất lượng của hệ thống, và một phép đo của một loạt các mẫu thủy tinh như làsử dụng thực tế của nó.

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A practical test of a c–c coincidence measurement setup for PGAA

P.P Ember *, T Belgya, J.L Weil, G.L Moln a ar

Institute of Isotope and Surface Chemistry, Chemical Research Centre of the Hungarian Academy of Sciences,

P.O Box 77, H-1525 Budapest, Hungary

Abstract

A second cold-neutron beam experimental station has been built as part of the renewal of our prompt gamma activation analysis facility at the Budapest Research Reactor This new station has been instrumented for neutron-induced prompt gamma-ray spectroscopy, involving c–c coincidence measurements The c–c coincidence arrangement

is introduced briefly, and its usage is illustrated with a practical example of the inactive tracer method for samples from glass furnace

 2003 Elsevier B.V All rights reserved

PACS: 25.40.Lw; 81.70.Jb; 82.80.Ej; 82.80.Jp

Keywords: ðn; cÞ; E n ¼ cold; Prompt gamma activation analysis; Coincidence; Spectral interference

1 Introduction

The c–c coincidence method (detection of two c

rays emitted almost simultaneously) has been used

in nuclear structure studies [1], and is also a

pos-sible way to improve the sensitivity of the prompt

gamma activation analysis (PGAA) technique [2]

As part of the facility for neutron-induced

prompt gamma-ray spectroscopy (NIPS) at the

PGAA beam port of the Budapest Research

Reac-tor a c–c coincidence apparatus has been developed

In our previous articles the regional c–c

coin-cidence method was introduced [2], and the

mea-surement setup was described in detail [3] In our

present article we show a chlorine measurement to

illustrate the quality of the system, and a mea-surements of a series of glass samples as the first practical usage of it

2 Experimental work All measurements were made using the same arrangement, as detailed in our most recent article [3]

2.1 Detector parameters and positioning Two coaxial HPGe detectors were used for the measurements described here Detector HPGe-I had 30% efficiency relative to a 300· 300NaI detector and 1.8 keV resolution at 1332 keV c-ray energy Detector HPGe-II had 15% efficiency and 1.9 keV resolution HPGe-II was placed horizontally at a

*

Corresponding author Fax: +36-1-392-2584/2222.

E-mail address: ember@alpha0.iki.kfki.hu (P.P Ember).

0168-583X/$ - see front matter  2003 Elsevier B.V All rights reserved.

doi:10.1016/S0168-583X(03)01663-X

Nuclear Instruments and Methods in Physics Research B 213 (2004) 406–409

www.elsevier.com/locate/nimb

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distance of 4.3 cm from the target, and HPGe-I

vertically, about 2.6 cm from the target Lead

blocks of 5 cm thickness were used around the

crystals as gamma shields, and plates of 1.5 mm

thick lead were placed between the detectors and

the tube to decrease the number of back-scattered

gamma photons, and to filter out the X-rays

2.2 Test samples

The chlorine sample was a PVC foil of 0.11 g

mass and 1.8· 2.5 cm2 surface area It was

irra-diated in the neutron beam for 23 h to excite the

36Cl nuclei via the 35Cl(n,c) reaction, which has a

large cross section The de-exciting c-rays have

been measured in coincidence mode

The glass samples were borrowed from a series

of industrial measurements carried out with the

Compton-suppressed spectrometer at our PGAA

facility [4,5] Recently a series of experiments were

performed to measure the uniformity of mixing of

input ingredients in a glass furnace with an

inac-tive tracer method This furnace works

continu-ously, and the tracer was injected in an instant

with the ingredients, and the samples were taken at

certain times from the outcoming melted glass

The process is shown in Fig 1 Important aspects

of the tracer selection were: it should not affect the

technology, nor change the parameters of the

produced glass Furthermore it has to have a large

neutron capture cross section Boron was selected

for normal glasses, and gadolinium for the

bo-rosilicate glasses containing approximately 5% of

boron Our samples were taken from a

measure-ment series of borosilicate glasses The original

samples were of several tens of grams, thus we cut

from them about a half gram for our purpose

Table 1 contains the data of the four glass samples: the number of the sample for reference, the mass of the borated glass sample (used for the coincidence measurement), the measuring time (equals with the irradiating time), and the Gd concentration with its uncertainty The concen-tration data were calculated from the Compton-suppressed measurement Sample 0 was taken just before the gadolinium tracer was put into the furnace, so this measurement represents the natu-ral gadolinium concentration of the glass

3 Results and discussion 3.1 Chlorine sample

48 million coincidence events were collected in the chlorine experiment The upper half of Fig 2 shows the total projected time spectrum, which means the histogram of all time values from the list

Fig 1 Draft of the inactive tracing of a glass furnace.

Table 1 Data of the glass samples Sample number 0 1 2 4 Sample mass (g) 0.529 0.536 0.449 0.48 Measuring time (min) 1052 1179 1220 325

Gd concentration (ppm) 0.87 1.4 11.9 21.9 Uncertainty of Gd

con-centration (ppm)

0.1392 0.106 1.547 1.533

Gd concentration was measured by the Compton-suppressed PGAA spectrometer of the NIPS facility.

Fig 2 Time spectrum of 60Co c–c coincidence events Gates were set on the 1173 and 1332 keV c peaks in the HPGe-I and HPGe-II energy spectra respectively.

P.P Ember et al / Nucl Instr and Meth in Phys Res B 213 (2004) 406–409 407

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file The time spectrum has a peak to background

ratio of 150, and FWHMof 30 ns The structure of

any time spectrum depends on many factors, such

as the detector dimensions, the threshold setting in

the CFD electronics, and the variety of transition

energies and life times of levels involved in the

de-excitation process of the target nuclei In the case

of a broad energy range of transitions, one cannot

obtain as good time resolution as can be obtained

with e.g a 60Co-calibration source [3] and narrow

energy gates, due to the time-walk of the detector

output signals [6] In addition, finite lifetimes cause

centroid shifts or exponential tails that also

broaden the time peak The lower half of Fig 2

illustrates the time walk by showing the time peak

of three full energy peak-to-peak coincidences In

detector HPGe-I a gate on the 517 keV energy

peak was set for all three cases, while in HPGe-II

gates on the 6110, 1951 and 786 keV peaks were

applied respectively The effect of the time walk is

clearly visible; the stop signals of higher energy

(higher amplitude) pulses come earlier, while the

lifetimes of the intermediate levels are negligible

The measured FWHMvalues of the three time

peaks are 13 ns, which is the same as was found for

the60Co time peak [3]

Fig 3 presents the total projection of the

HPGe-I detector energy signals from the35Cl(n; c)

capture reaction As can be seen, a few very strong

lines dominate the spectrum, including the

strongest primary transition of 6110 keV energy

For demonstration of the off-line coincidence

analysis method, we set a gate on the 5086 keV double escape peak, instead of the 6110 keV full energy peak, because the latter and its single es-cape peak form doublets with the single- and double-escape peaks of a weaker, higher energy c ray To estimate the background, we set back-ground regions on both sides of the time and en-ergy peaks The peak and background gate settings are shown as gridded and crosshatched areas, re-spectively, in Fig 3 The two background regions combined cover the same number of channels as the peak gates The analysis program subtracts the projection of the backgrounds automatically from the coincidence projection spectra and also calcu-lates the uncertainties in the gated spectrum

In Fig 4 the spectrum of the c-rays measured

by the HPGe-I detector with the gate settings ex-plained above is shown The strongest coincidence peaks are labeled with their energies As can be seen, the signal to noise ratio is very good The random coincidences have almost completely dis-appeared, as illustrated by the magnified insert of the energy-gate setting area Fig 5 shows the corresponding decay scheme (taken from ENSDF [7]) for the 35Cl(n; c)36Cl reaction, retaining only those transitions which are expected to be in co-incidence with the strongest 6110 keV primary capture c-ray For easier reading the c-ray energies and their absolute intensities in percentage are rounded off The c transitions with intensity less than 1% are drawn with dotted lines

Fig 3 Total projection energy spectrum of the HPGe-I

de-tector from the chlorine experiment.

Fig 4 Spectrum of c-rays in coincidence with 5086 keV, the double escape peak for 6110 keV.

408 P.P Ember et al / Nucl Instr and Meth in Phys Res B 213 (2004) 406–409

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In agreement with our expectations, the gated

energy spectrum of HPGe-II contains only the

peaks expected from the known level scheme of

36Cl The weak 2467 keV line can be easily

iden-tified, but the 511 keV annihilation peak masks the

similarly weak 508 keV line

3.2 Glass samples

The above outlined c–c coincidence technique

was applied for the analysis of the glass samples

The peak areas were normalized for each sample

to 1 g sample mass and 1000 min of measurement

time

Fig 6 shows the calibration curve for the

co-incidence measurement: the calculated and

nor-malized peak areas for the 182 keV gadolinium

peak are plotted versus the gadolinium

concen-tration calculated from the Compton-suppressed measurements Each point has the uncertainty marked in both directions The graph also shows the fitted linear function that was forced to cross the origin The r2value of the fit is also given on the graph As can be seen in Fig 6 the calibration curve is linear, which means the method is appli-cable for concentration determination

4 Conclusions

In this article we have studied the applicability

of c–c coincidence for the determination of con-centrations with PGAA method We found that the coincidence reduces spectral background and interference, but preserves the linear relationship between signal and concentration A possible way

of further improvement is the use of a digital signal analyzer, which would allow larger count rates, and hence better precision for a given measuring time

References

[1] A.H Wapstra, Alpha and Gamma-ray Spectroscopy, Vol I, fifth printing, North Holland Publishing Company, Am-sterdam New York Oxford, 1979, Chapter VIII/C, p 539 [2] P.P Ember, T Belgya, G.L Moln a ar, Appl Radiat Isot 56 (2002) 535.

[3] P.P Ember, T Belgya, J.L Weil, G.L Moln a ar, Appl Radiat Isot 57 (2002) 573.

[4] T Belgya, Zs R eevay, B Fazekas, I H eejja, L Dabolczi, G.

L Moln a ar, Z Kis, J € O Ost€ o or, Gy Kasz a as, in: Proceedings of the Ninth International Symposium on Capture Gamma-Ray Spectroscopy and Related Topics, Vol 2, Budapest, Hungary, 1996, p 826.

[5] G Moln a ar, T Belgya, L Dabolczi, B Fazekas, Zs R eevay,

 A

A Veres, I Bikit, Z Kiss, J € O Ost€ o or, J Radioanal Nucl Chem 215 (1997) 111.

[6] G.F Knoll, Radiation Detection and Measurement, third ed., John Wiley & Sons, New York, 2000, Chapter 17/IX,

p 438.

[7] Evaluated Nuclear Structure Data File (ENSDF) produced

by members of the International Nuclear Structure and Decay Data Network, and maintained by the National Nuclear Data Center, BNL, USA Also available online from IAEA Nuclear Data Section Vienna.

Fig 5 Partial decay scheme of 36 Cl Only the lines in

coinci-dence with the 6110 keV peak are shown.

Fig 6 Calibration curve for the 182 keV chlorine peak.

P.P Ember et al / Nucl Instr and Meth in Phys Res B 213 (2004) 406–409 409

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