A gamma-gamma coincidence spectrometer for nuclear attribution and safeguard applications
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1 IAEA-CN-184/174 A gamma-gamma coincidence spectrometer for nuclear attribution and safeguard applications Weihua Zhang, Jing Yi, Pawel Mekarski and Kurt Ungar Radiation Protection Bureau of Health Canada, 775 Brookfield Road, Ottawa, Ontario, K1A 1C1 Canada Abstract This paper reports on initial efforts for uranium isotopic analysis using gamma-rays and X-ray fluorescence coincidence. In this study, a gamma gamma coincidence spectrometry was developed. The spectrometry consists of two NaI(Tl) scintillators and XIA LLC Digital Gamma Finder (DGF)/Pixie-4 software and card package. The developed spectrometry was optimized according to the considerations of output count rate and gamma peak energy resolution. It has been demonstrated that the spectrometry provides an effective method of assessing the content of uranium isotopes for nuclear materials. The main advantages of this approach over the conventional gamma spectrometry include that the 235 U enrichment can be graphically characterized by their unique coincidence fingerprint. The method could be further developed for fast uranium isotope verification with an established gamma-gamma coincidence spectral imaging library by various nuclear materials. 1. Introduction In this study, gamma-gamma coincidence spectrometric method has been developed and proposed for rapid isotope screening of nuclear and radiological materials. The focus of this study is to establish a methodology that enables rapid identification of uranium enrichments by three dimensional gamma-gamma coincidence graphical signatures of uranium isotopes, and quantification of uranium isotopes with minimal calibrations. There are several advantages of the method over the conventional gamma spectrometry for uranium isotopic analysis. First, it has a low background continuum near coincident signatures due to the requirement of having coincident photon energy deposited in two detectors. The uranium gamma-gamma coincidence event becomes the dominant signal in the determined spectrum. Second, gamma-gamma coincident counting eliminates many of the interferences that are presented in conventional gamma spectrometry, such as gamma-ray of 226 Ra. Finally, the study has demonstrated that three dimensional gamma-gamma coincidence spectrum measured by the method can be used as a graphic pattern or fingerprint to distinguish the uranium enrichment in nuclear materials. Thus it is possible to determine if a sample has enriched uranium by pattern recognition and image analysis. 1
2 2. System descriptions and calibrations The gamma gamma coincidence spectrometry consists of two cm NaI(Tl) scintillators with their endcaps facing each other and the endcap-to-endcap distance is continuously adjustable. A sample can be positioned in the middle of two detectors for counting. This orientation provides a large geometric efficiency when the two detector distance is small; and this configuration provides maximum cross-talks probability. These cross-talks, resulting from coincident backscattered of the kev gamma-ray of 235 U, can be used to quantify and qualify the 235 U enrichment in nuclear material. The NaI(Tl) was selected because of its satisfied energy resolution at a reasonable cost. Each NaI(Tl) detector is a combination of scintillator/photomultipier (PMT) and preamplifier manufactured by Bicron (Saint Gobain), Newbury. The PMT high-voltage power supply is a programmable DC power supply from National Instruments, Austin, model number NI PXI The preamplifier is powered by an ORTEC portable power supply, with model number 4002P. The data-acquisition system for the spectrometer utilizes all-digital electronics, based on the X-Ray Instrumentation Associates (XIA LLC) Digital Gamma Finder (DGF)/Pixie-4 software and card package [1]. The Pixie-4 card is a four channel digital pulse-processing module deployed on a chassis with CompactPCI/PXI backplane from National Instrument. The waveform of an input signal, taken directly from NaI(Tl) preamplifier output, is continuously sampled and digitized by a 14-bit analog-to-digital converter (ADC) at a rate of samples/s. The signal pulse height is determined by a programmable, digital trapezoidal energy filter implemented in a field-programmable gate array (FPGA). Preamplifier pulse heights are determined to 16-bit resolution. Event timing and pulse-pileup inspection is also carried out in the FPGA by a fast programmable trapezoidal trigger filter. Events are time-stamped at the full ADC rate of 75 MHz. The Pixie-4 card resides in a 4-unit PXI crate. A host desktop PC controls the pulse processing module and performs data readout. All operating parameters, including the filter values, are user adjustable in the software on the host PC. The coincidence time window is also set in the software with a step of ns and a lower limit of ns, thus allowing accurate reconstruction of coincident interactions in two NaI(Tl) detectors. The parameters of trapezoidal trigger and energy filter, such as trigger threshold, filter rise and flat top time, are optimized by maximizing the output and input count rate ratio and minimizing the kev peak resolution of 137 Cs. Whenever a valid event is detected, a digital signal processor (DSP) reads out the energy filter values, reconstructs the pulse height, and bins the energy. In the case of coincidence counting, the DSP obtains the coincidence pattern of active channels in a given event. The simplicity of the present coincidence system is especially apparent in contrast to the systems associated with many NIM-based analog processing modules [2]. Three certified standard point sources ( 241 Am, 137 Cs and 22 Na) from Eckert & Ziegler Analytics were used for the energy and energy resolution calibrations of each NaI(Tl) scintillator. The calibration data are listed in Table 1. By tuning each PMT s high-voltage supply, and gain, and offset of each Pixie-4 card input channel, the same full-energy gamma ray appears in almost the same center channel for both NaI(Tl) detectors. The 2
3 energy resolution of the two NaI(Tl) detectors is around 7% at kev, which is very close to each other. 3. Samples The samples used for the study were National Bureau of Standards (NBS) SRMs U950b (NU), U0002 (DU), U100 (LEU), U800 (HEU) and a weapons-grade metallic uranium sample. The reference materials consist of normal uranium in the form of oxide, U 3 O 8, with uranium oxide mass fraction more than 99.9%. The uranium molar mass used in the NBS U950b calculation was g/mol, suggesting an isotopic abundance of 235 U in the range %, which is close to natural isotopic composition. The certified 235 U enrichment of U0002, U100 and U800 are 0.02%, 10% and 80% respectively. The mass of each sample was about 1 g, and introduced onto the bottoms of cylindrical glass vials, forming disks of approximate dimensions 1.55 cm dia cm height for counting. The metallic uranium sample was obtained from a nuclear forensic laboratory HEU characterization exercise. It was approximately in cylindrical pellet form with a 0.25 cm dia cm height. Its uranium concentration was determined by more than 99.9% by weight. The sample was weighted about 0.16 g, and introduced onto the bottoms of a small plastic vial for counting. 4. Results and discussion The composition of the NBS standards was mainly 235 U and 238 U. Most of the visible gamma-rays are from 235 U, 234 Th and 234m Pa (progenies of 238 U) and X-ray fluorescence. For each NBS standard, list-mode data were collected by the gamma-gamma coincidence counting system over 600 seconds at a ns coincidence window. The data acquired in list-mode includes coincidence events consisting of records of energy in DSP units and timestamp from NaI(Tl) detector A and B. The list-mode data was stored in a text file for offline analysis. During offline analysis, the DSP units of coincidence events from both NaI(Tl) detectors A and B were divided by detector s calibration factor correspondingly, then a histogram was created of the three-dimensional (3D) gammagamma coincident energy spectrum. The U950b standard contains 99.28% 238 U and 0.72% 235 U. Most of the radiation originates from 238 U, 234 Th, 234 Pa, 234m Pa and U K-shell X-ray fluorescence. The gammagamma coincidence 3D spectrum collected, shown in Figure 1, displays the most intensive ROI-e resulting from U-K α and U-K α coincidences in both detectors. The X- rays (94.7 and 98.4 kev) are self-excited fluorescence by inner radiations in the uranium material in the presence of other uranium atoms near the location of the decay [3]. The yields of the self-excited X-ray fluorescence are more than 30% allowing a more intensive coincidence peak to be observed. The two ROI-b regions lined up diagonally are mainly results of detectors cross-talks of kev gamma-ray of 235 U. Other gamma-rays of 235 U, may also have contributions for this coincidence counts because of low resolution of NaI(Tl) detector. The vertical and horizontal tailings (ROI-f) are due to random coincident events between U-K α deposited in one detector and X-ray fluorescence continuous (bremsstrahlung radiation) deposited in the other. The two 3
4 diagonal tailings are caused by bremsstrahlung radiation coincidence of two detectors. The ROI-d arise from the coincidence of kev gamma-ray deposited in one detector and kev gamma-ray of 234m Pa measured in the other. Figure 1: Top view of the determined 3D histogram of U950b NU standard obtained by one hour counting. At elevated 235 U concentrations, the determined 3D coincidence spectrum apparently has different features. As shown in Figure 2 (a), the coincidence spectrum obtained by U200 (LEU) shows relative weak coincidence tailings resulting from bremsstrahlung radiation and a feeble coincidence peak between kev and kev gamma-ray of 234m Pa (ROI-d). Other coincidence counting with U100, U800 and U930d indicate that the higher 235 U enrichment, the shorter the bremsstrahlung radiation coincidence tailing and the less coincidence events in ROI-d. Other coincidence counting with U100, U800 and U930d indicate that the higher 235 U enrichment, the shorter the bremsstrahlung radiation coincidence tailing and the less coincidence events in ROI-d. As an example, the coincidence spectrum obtained by U930d is given in Figure 2 (b). These observations may be explained by the fact that the strong kev gamma-ray from 235 U excites Th K-shell X-rays from the thorium (daughter of uranium) much more efficiently at 235 U high enriched samples. The Th K-shell excited X-rays may have much less chance to 4
5 produce coincident events with bremsstrahlung radiation that mainly generated by the X- ray excitation of 238 U and its progenies. As the 235 U enrichment increased to 80% (U800), coincidence events in the ROI-d resulting from 238 U become very week. Figure 2: Top view of the determined 3D gamma-gamma coincidence spectrum of U200 LEU with one hour counting (a); and U930d HEU with 600 seconds counting (b). 5. Conclusions and future work The results obtained so far have shown that the gamma-gamma coincidence spectrometry is a relatively simple technique that would allow for the counting and monitoring the content of uranium isotopes of nuclear materials. The experiment showed that the spectra of natural and depleted uranium materials is characterized by coincidence tailings between U K-shell fluorescent X-rays and 234 Pa beta-decay produced bremsstrahlung radiation. The coincidence spectra of 235 U enriched and weapons-grade materials is dominated by detectors cross-talks of kev gamma-ray of 235 U and the coincidence between K-shell X-ray and K-shell X-ray sum peaks. It was also shown that the relative intensity of L-shell and K-shell X-ray coincidence peak to K-shell and K-shell X-ray coincidence peak allows an estimation of properties of uranium matrix composite. Future development of the method includes developing a protocol that enables an automated recognition of uranium isotope enrichment and specific substances with an established gamma-gamma coincidence spectral imaging library by various nuclear materials. 5
6 6. References [1] Hennig W, Chua YX, Tana H, Fallu-Labruyerea A, Warburtona WK and Grzywaczb R, The DGF Pixie-4 spectrometer: compact digital readout electronics for HPGe clover detectors, 2007, Nucl Instrum Methods Phys Res Sect B Inter Mater Atoms 263(1): [2] Weihua Zhang, Jing Yi, Pawel Mekarski, Ian Hoffman, Kurt Ungar and Ari-Pekka Leppanen, A system for low-level the cosmogenic 22 Na radionuclide measurement by gamma gamma coincidence method using BGO detectors, 2010, J. Radioanal. Nucl. Chem., DOI /s [3] Dragnev, T., Rukhlo, V., Rundquist, D., Szabo, E., Combined Gamma and passive X- ray fluorescent measurement of 235 U enrichment and U-total concentration, 1991, Journal of Radioanalytical and Nuclear Chemistry, 152(1),
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