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104 records · Page 6

Growth of Cd 0.9 Zn 0.1 Te 1-y Se y Single Crystals for Room Temperature Gamma-Ray Detection

Quaternary Cd 0.9 Zn 0.1 Te 1-y Sey (CZTS) single crystals, a novel room-temperature nuclear radiation detector semiconductor material, have been grown using a modified vertical Bridgman method (VBM) and a travelling heater method (THM). The percentage concentration of selenium in the VBM-grown crystal was 3% and that in the THM-grown crystal was 2%. While the THM Frisch collar detector (4.4 × 4.4 × 10.7 mm 3 ) produced a highly resolved pulse height spectra (PHS) with a resolution of ~1.06% for 662-keV gamma rays without any correction, the VBM-grown detector (10 × 10 × 2 mm 3 ) offered a high energy resolution of ~2% after application of a digital biparametric correction. The high-resolution performance of these detectors has been attributed to the addition of Se in the Cd 0.9 Zn 0.1 Te (CZT) matrix. Ab-initio calculations based on density functional theory (DFT) also confirmed that the addition of Se in the CZT matrix helps to reduce the formation of TeCd and the TeZn anti-sites. The VBM-grown crystals were characterized using powder x-ray diffraction (XRD) and energy dispersive x-ray spectroscopy (EDS). While XRD results revealed sharp diffraction peaks confirming the crystalline nature of the grown crystal, the EDS results confirmed the targeted stoichiometry of the elemental composition. The bulk resistivity of the grown crystal was calculated to be ~3 × 10 10 Ω-cm from current-voltage characteristics recorded at room temperature in a planar configuration, ensuring that the grown CZTS crystals have low dark current as required for detector-grade crystals.

42 ENGINEERING↗

Effects of excess Te on flux inclusion formation in the growth of cadmium zinc telluride when forced melt convection is applied

The presence of second phase defects, particularly flux inclusions of tellurium rich composition, are of great concern for charge collection efficiency in cadmium zinc telluride (CZT) and cadmium telluride (CT) material intended for applications such as radiation detection. These inclusions can distort applied electric field lines within the detector as well as act as trapping centers for charge carriers. Reduction and/or elimination of these inclusions is required to achieve appropriate charge collection efficiencies, especially in detectors of thicknesses greater than 5 mm. These so-called flux inclusions are understood to form as a consequence of constitutional undercooling at the crystal growth interface. In this study, a forced melt convection technique was applied in Vertical Bridgman (VB) melt growth of CZT without reducing imposed growth rates of ~2 mm/hr. Several rotation profiles were tested while adjusting the melt composition from 51.62 to 61.75 atomic percent (at%) Te where the Te concentration was initially increased to improve overall material purity. With forced melt convection, the best inclusion distributions were achieved with highly Te rich melt compositions, far beyond the stoichiometric composition range for the CZT system. Average inclusion diameters were reduced to 2 µm while inclusions greater than 5 µm were essentially eliminated. Composition analyses of these ingots revealed near equilibrium concentrations of Te, even with ingots grown from Te concentrations as high as 61.75 at% Te. In this paper, a recipe for the reduction of inclusions in CZT melt growth is put forward and the implications of this method on our understanding of inclusion formation are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effect of Surface Passivation of CZTS Semiconductor Detector on Leakage Current

Cadmium Zinc Telluride Selenide (CdZnTeSe or CZTS)has shown high crystal quality for room-temperature gamma ray and X-ray detection applications compared to Cadmium Zinc Telluride (CdZnTe or CZT) [1,2]. Current applications of CZT include medical imaging, homeland security, and X-ray and gamma ray astronomy [3]. CZST has similar potential applications

Kangethe, Anthony [Morgan State Univ., Baltimore, ↗

Machine learning framework for predicting uranium enrichments from M400 CZT gamma spectra

A machine learning framework was developed for predicting uranium enrichments from M400 CZT gamma spectra. This framework leverages the availability of a large amount of measured M400 gamma spectra and uses a recently updated version of Gamma Detector Response and Analysis Software (GADRAS) for gamma spectrum analysis and generation. It also leverages the existing machine learning modules in Python for gamma spectrum data processing, curation, model training, benchmarking, and optimization of the deep machine learning models. The framework is used to develop a deep learning model to analyze gamma spectra from a set of U 3 O 8 samples with enrichments ranging from 0.31 to 93.17% and UF 6 cylinders with enrichments ranging from 0.2 to 4.95%, and the model performance is tested using a set of measured spectra and the respective declared enrichment values. Results show that the model can correctly classify 99.35% of the U 3 O 8 sample enrichments, and can predict the samples’ enrichments within an average absolute error of 0.099% (in percentage points of enrichment). For the UF 6 cylinders, the average absolute error was approximately 0.03%, with an accuracy of 98% in classifying discrete enrichment values of UF 6 samples. Finally, the results also show that the model has performed significantly better in terms of predicting enrichments in UF 6 cylinders based on measured gamma spectra than the GEM code, with a standard deviation (of the relative errors) of 2.23% (compared with the 11.51% value for the GEM code) based on results from a set of test data.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Development of a Silicon Tracker for the All-Sky Medium Energy Gamma-ray Observatory Prototype

The gamma-ray sky from several hundred keV to a hundred MeV has remained largely unexplored due to the challenging nature of detecting gamma rays in this regime. At lower energies, Compton scattering is the dominant interaction process whereas at higher energies pair production dominates, with a crossover at a few MeV. Thus, an instrument designed to work in this energy range must be optimized for both Compton and pair-production events. AMEGO, the All-sky Medium Energy Gamma-ray Observatory, a Probe-class mission in consideration for the 2020 decadal survey, is designed to operate at energies from 200 keV to > 10 GeV with over an order of magnitude increase in sensitivity and with superior angular and energy resolution compared to previous instruments. AMEGO comprises four major subsystems: a plastic anticoincidence detector for rejecting cosmic-ray events, a silicon tracker for tracking pair-production products and tracking and measuring the energies of Compton-scattered electrons, a cadmium-zinc-telluride (CZT) calorimeter for measuring the energy and location of Compton scattered photons, and a CsI calorimeter for measuring the energy of the pair-production products at high energies. A prototype instrument, known as ComPair, is under development at NASA’s Goddard Space Flight Center and the US Naval Research Laboratory. In this contribution, we provide details on the development of the silicon tracker subsystem.

Griffin, Sean↗

Data-Driven Performance Optimization of Gamma Spectrometers With Many Channels

In gamma spectrometers with variable spectroscopic performance across many channels (e.g., many pixels or voxels), a tradeoff exists between including data from successively worse-performing readout channels and increasing efficiency. Brute-force calculation of the optimal set of included channels is exponentially infeasible as the number of channels grows, and approximate methods are required. In this work, we present a data-driven framework for attempting to find near-optimal sets of included detector channels. The framework leverages non-negative matrix factorization (NMF) to learn the behavior of gamma spectra across the detector and clusters similarly-performing detector channels together. Performance comparisons are then made between spectra with channel clusters removed, which is more feasible than brute force. The framework is general and can be applied to arbitrary, user-defined performance metrics depending on the application. We apply this framework to optimizing gamma spectra measured by H3D M400 CdZnTe (CZT) spectrometers, which exhibit variable performance across their crystal volumes. In particular, we show several examples optimizing various performance metrics for uranium and plutonium gamma spectra in non-destructive assay (NDA) for nuclear safeguards, and explore trends in performance versus parameters such as clustering algorithm type. We also compare the NMF + clustering pipeline to several non-machine-learning (ML) algorithms, including several greedy algorithms. Although, we find that the NMF + clustering pipeline tends to find the best-performing set of detector voxels, significantly improving over the unoptimized spectra, but that a greedy accumulation of spectra segmented by detector depth can, in some cases, give similar performance improvements in much less computation time.

Energy resolution↗

Gamma Spectrometry Code Rodeo for Uranium Enrichment—FY 2021 Report

In FY22, the participating Department of Energy (DOE) laboratories continued the work on the project “Gamma Spectrometry Code Rodeo for Uranium Enrichment”. Oak Ridge National Laboratory (ORNL) and Lawrence Livermore National Laboratory (LLNL) continued their efforts to acquire spectra using uranium sources. A collimator (with side and back shields) was custom designed and constructed at ORNL. Spectra were acquired at ORNL using the uranium enrichment standards supplied by New Brunswick Laboratory (NBL) and the collimated M400 detector. Spectra were also acquired using steel absorbers of different thickness placed between the source and the collimated M400 detector. The plan was to ship the collimator to LLNL so that spectra could be acquired using the LLNL detector in collimated geometries. This activity was suspended since problems were noticed with the performance of the LLNL M400 detector. Also, it was brought to light to the project team that some of the aspects of the M400 detector had been updated by the vendor H3D in response to requests by the IAEA. In February 2021, the ORNL and LLNL M400 detectors were returned to the H3D factory in order to resolve the problems with the LLNL detector and to update ORNL and LLNL detectors to the same configuration as the M400 supplied to the IAEA. H3D repaired the LLNL M400 and performed the IAEA updates on both the ORNL and LLNL detectors. ORNL and LLNL received the detectors in April 2021. Data acquisition was continued using the upgraded detectors. ORNL re-collected the spectra using point sources and the NBL standards in uncollimated and collimated geometries. The collimator was shipped from ORNL to LLNL. Spectra were acquired at LLNL through Q4 of FY22. When the ORNL spectra were examined closely, it became apparent that there were spurious artifacts present in some of the spectra. This rendered suspect the ORNL spectra collected in June/July 2021 time frame. ORNL contacted H3D and per H3D’s advice, the M400 detector was returned to H3D for repairs in mid-August 2021. H3D diagnosed the problem and established that the root cause was the extra tight packaging that created a strain on the CZT crystals, causing one of them to break down. The repaired M400 was returned to ORNL in early September 2021. ORNL re-started data acquisition for the third time. Data was continued to be acquired at ORNL and LLNL through September 2021. The ORNL and LLNL data will be shared with the principal investigators from the analyzing laboratories. The GADRAS code and FRAM have been developed to have the capability to analyze the M400 spectra. Good quality spectra from FY21 have been analyzed using modified versions of GADRAS and FRAM. The spectra have also been analyzed using the GEM code. The analysis results from GADRAS, FRAM and GEM codes are presented and discussed in this report. Some preliminary results from FRAM and GEM analysis were presented in February 2021 at the U-Pu Isotopics Workshop sponsored by the IAEA. CZTU code is being modified to analyze M400 spectra. Data collection, code development and analysis will be continued in FY22 as per the FY22 Project Work Plan (PWP).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Gamma spectrometry uranium isotopic analysis rodeo: Summary of GADRAS results

This report summarizes GADRAS methods and gamma spectrometry rodeo uranium isotopic analysis results for high energy resolution H3D M400 cadmium zinc telluride (CZT) and ORTEC Micro Detective high-purity germanium (HPGe) spectra of uranium isotopic standards collected at Oak Ridge National Laboratory (ORNL) and Lawrence Livermore National Laboratory (LLNL) over a two-year measurement campaign. During the campaign, measurements were performed with the detectors unshielded, side shielded, and collimated. In addition, measurements of the uranium isotopic standards were performed unshielded and shielded.

07 ISOTOPE AND RADIATION SOURCES↗

CZT Imaging Arrays for Space Applications

The compound CZT offers great promise for space applications with applications in such areas as radiation monitoring, planetary investigations and astrophysics. As crystal quality improves, the challenge for imaging array development is to derive electrode geometries and readout electronics to satisfy particular applications and to understand how the material will perform in the space environment. An overview of present and future detector requirements will be given together with the status of current array developments.

Ramsey, Brian D.↗

Simulation studies of a full-ring, CZT SPECT system for whole-body imaging of 99m Tc and 177 Lu

Single photon emission computed tomography (SPECT) is an imaging modality that has demonstrated its utility in a number of clinical indications. Despite this progress, a high sensitivity, high spatial resolution, multi-tracer SPECT with a large field of view suitable for whole-body imaging of a broad range of radiotracers for theranostics is not available. With the goal of filling this technological gap, we have designed a cadmium zinc telluride (CZT) full-ring SPECT scanner instrumented with a broad-energy tungsten collimator. The final purpose is to provide a multi-tracer solution for brain and whole-body imaging. Our static SPECT does not rely on the dual- and the triple-head rotational SPECT standard paradigm, enabling a larger effective area in each scan to increase the sensitivity. We provide a demonstration of the performance of our design using a realistic model of our detector with simulated body-sized phantoms filled with 99m Tc and 177 Lu. Our SPECT design can resolve 7.9 mm rods for 99m Tc (140 keV) and 9.5 mm for 177 Lu (208 keV) in a hot-rod Derenzo phantom with a 3-min exposure and reach an image contrast of 78% for 99m Tc and 57% for 177 Lu using the NEMA IQ phantom with a 6-min exposure. Our modified scatter correction shows an improved contrast-recovery ratio compared to a standard correction. In this paper, we demonstrate the good performance of our design for whole-body imaging purposes. This adds to our previous demonstration of improved qualitative and quantitative 99m Tc imaging of brain perfusion and 123 I imaging of dopamine transport with respect to state-of-the-art NaI dual-head cameras. We show that our design provides similar IQ and contrast to the commercial full-ring SPECT VERITON for 99m Tc. Regarding 177 Lu imaging of the 208 keV emissions, our design provides similar contrast to that of other state-of-the-art SPECTs with a significant reduction in exposure. In conclusion, the high sensitivity and extended energy range up to 250 keV makes our SPECT design a promising alternative for clinical imaging and theranostics of emerging radionuclides.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fission Product Gas Monitoring During Fuel Drying Operations - 20094

The goal of the project was to devise and implement a method of accurately qualifying any noble gas emitted during fuel drying operations (part of the dry fuel storage process) in order to provide the data needed to validate the off-site dose calculations. The imputes of the project was the NRC publishing Information Notice 18-01, 'Noble Fission Gas Releases During Spent Fuel Cask Loading Operations' in February 2018. The information notice describes some industry events that occurred during vacuum drying operations as part of a dry fuel campaign. The solution was devised by Fort Calhoun Station staff in partnership with Mirion Technologies technical staff. The monitoring was accomplished by directing all the effluent from the fuel storage cask vacuum drying machine through a sample chamber containing a compact ISOCS characterized CZT based gamma spectrometer connected to a Mirion Data Analyst. This resulted near real-time quantification of the radionuclides of concern. (authors)

07 ISOTOPE AND RADIATION SOURCES↗

Photoluminescence of CdTe and CdZnTe compounds doped with 2% selenium

The addition of 2 % of selenium in CdTe and CdZnTe (CZT) exhibited an additional acceptor-bound exciton in photoluminescence (PL). From the PL and inductively coupled plasma mass spectrometer (ICP/MS) analyses, the additional acceptor-bound exciton emission is associated with a Cu impurity in the relatively low-purity (5N) precursor CdSe starting material. Additionally, thermal quenching of the acceptor/donor bound exciton emissions do not require a shift to any higher excited states or to the free exciton state. ICP/MS analysis also showed a higher concentration of Sn in CdZnTeSe (CZTS) compared to CdTe and CZT which is known to form a deep level trap at around E C – 0.83 eV. The trapping and de-trapping times indicate that the Sn-related deep trap acts as an electron trapping center. The relatively low electron mobility-lifetime product of CZTS might be correlated with the concentration of Sn in the impure CdSe material. Pulse height spectra using an Eu-152 gamma-ray source was taken for a 2-mm-thick planar CZTS detector. The spectra clearly showed all the expected gamma peaks with energy lower than 344.3 keV.

47 OTHER INSTRUMENTATION↗

Quantification of LEU Holdup using gamma ray imaging and inverse transport solver

Holdup is the residual amount of special nuclear material (SNM) remaining in a processing facility after the bulk materials have been cleaned out. In commercial uranium processing facilities, quantification of holdup is a major challenge because of the highly variable shapes and sizes of the deposits. Any method that attempts to generalize and calibrate deposit shapes in order to quantify holdup will be prone to high uncertainties. Uncertainties on the order of ±50% are typical in holdup results. In international safeguards applications, a ±50% uncertainty can result in a large amount of material unaccounted for (MUF) thereby increasing the difficulty of detecting material diversion and facility misuse. An imaging-based methodology has been developed with the objective of significantly reducing this uncertainty by using the true deposit shape, instead of relying on oversimplified geometric assumptions. The project is a collaboration between ORNL, Y-12, and the University of Tennessee, Knoxville, TN. Uranium sources of known masses were measured using the Germanium Gamma-ray Imager (GeGI), a high-resolution imaging spectrometer, creating a pixelated map for each spectral bin. Two different gamma imaging methods are employed in this work: coded aperture imaging and Compton imaging. A validated MonteCarlo model of the detector has been developed using the GEANT4 code for determining the intrinsic response of the detector, its enclosure, and the coded aperture mask. An inverse transport solver based on the Markov Chain Monte-Carlo approach known as Differential Evolution Adaptive Metropolis (DREAM) is employed to use the measurement data from the image pixels (coded aperture or Compton) to solve for the mass of 235 U in the deposit. A reliable method based on the DREAM solver has been developed to flag the infinite thickness condition of a uranium deposit. The project team is working towards improving the image reconstruction for Compton imaging so that a better localization of the source can be achieved. Besides treating the coded aperture and Compton imaging methods independently, the project is also evaluating a combined method that uses the Compton scatter data from a coded aperture measurement. GEANT4 simulations are being performed to evaluate the combined approach. The impact on the DREAM optimization as the source thickness progressively approaches infinite thickness is being evaluated. A number of uranium sources available at ORNL have been measured, and the DREAM results have been tested and validated for the coded aperture imaging. A similar effort will be carried out to validate the Compton based method once the development of algorithms for better localization are complete. The imaging based quantification is very amenable to unattended monitoring of holdup accumulation at key measurement points. A proof of concept measurement has been completed to demonstrate this capability The current work used the high energy resolution imager GeGI. However, the approach and methodologies are applicable to other imagers such as the cadmium zin telluride (CZT) based imager manufactured by H3D, Inc.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗