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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Extreme γ –Ray Radiation Tolerance of Spectrometer–Grade CsPbBr 3 Perovskite Detectors

The perovskite compound CsPbBr 3 has recently been discovered as a promising room-temperature semiconductor radiation detector, offering an inexpensive and easy-to-manufacture alternative to the current benchmark material Cd 1–x Zn x Te (CZT). The performance of CsPbBr 3 sensors is evaluated under harsh conditions, such as high radiation doses often found in industrial settings and extreme radiation in space. Results show minimal degradation in detector performance after exposure to 1 Mrad of Co-60 gamma radiation, with no significant change to energy resolution or hole mobility and lifetime. Additionally, many of the devices are still functional after being exposed to a 10 Mrad dose over 3 days, and those that do not survive can still be refabricated into working detectors. Notably, these results suggest that the failure mode in these devices is likely related to the interface between the electrode and material and their reaction, or the electrode itself and not the material itself. Overall, the study suggests that CsPbBr 3 has high potential as a reliable and efficient radiation detector in various applications, including those involving extreme fluxes and energies of gamma-ray radiation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Optimizing $\mathrm{ACRT}$ to reduce inclusion formation during the $\mathrm{VGF}$ growth of cadmium zinc telluride: II. Application to experiments

Here two different accelerated crucible rotation technique (ACRT) rotation schedules are assessed, via theoretical computations and growth experiments, according to their ability to reduce tellurium-rich inclusions during the vertical gradient freeze (VGF) of cadmium zinc telluride (CZT). A vigorous rotation schedule based on classical ACRT guidelines produces a well-mixed melt that is expected to reduce tellurium inclusions compared to growth without crucible rotation. In contrast, a new ACRT schedule, derived from model-based optimization for interface stability, employs slower rotation with longer periods and is predicted to further reduce inclusions. Growth experiments corroborate these expectations. Namely, both ACRT schedules result in crystals with inclusion size and volume significantly decreased from levels found in material grown with no rotation, and material grown using the computationally optimized ACRT parameters exhibits a median inclusion size that is smaller and with a sharper distribution than in material grown via classical ACRT.

36 MATERIALS SCIENCE↗
DOE OSTI2025

X-ray escape peaks in gamma-ray spectrum acquired by perovskite detector

The X-ray escape peaks are clearly visible in the high-resolution gamma spectra acquired by CsPbBr 3 , credit to the rapidly improving energy resolution of perovskite gamma detectors. But it also raises concerns. If this peak remains as significant as it is, perovskite gamma detectors would have very limited use in complex gamma spectrometry applications. This paper discusses the origin of the escape peaks in CsPbBr 3 detectors, benchmarked against Ge and CZT detectors. The Pb escape peak consists of four escape peaks that are merged together, while the Cs and Br escape peaks are hidden inside the photopeak of 137 Cs (662 keV). These combined effects either create a noticeable gamma peak observed to the left of the 662 keV photopeak when acquired using a high-resolution CsPbBr 3 detector or raise the left slope of the photopeak. We also explore potential methods to mitigate these peaks, such as applying anti-coincidence method. The height of the escape peaks diminishes as the detector volume increases but will not go away entirely. The relationship between the observed Pb escape peak and the detector's dimensions is demonstrated through Monte Carlo simulation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Growth of High-Purity CsPbBr 3 Crystals for Enhanced Gamma-Ray Detection

High-quality CsPbBr 3 crystals hold significant potential for gamma-ray detection due to their remarkable optoelectronic properties. This study details an optimized production process using the Bridgman method to achieve highly pure CsPbBr 3 crystals. By implementing rigorous synthesis and purification techniques, we successfully reduced the total impurity levels to 9 ppm, as confirmed by glow discharge mass spectroscopy (GDMS). The resulting CsPbBr 3 crystals demonstrate exceptional performance, including high transparency, intense photoemission, and prolonged photoluminescence decay times. These properties facilitate superior gamma-ray detection with an energy resolution of 1.4% for the 137 Cs 662 keV gamma-rays, comparable to commercial Cd 1-x Zn x Te (CZT) detectors. Our findings underscore the critical relationship between material purity and detector performance, highlighting the potential of CsPbBr 3 as a cost-effective alternative in radiation detection applications. Further studies on defect origins and electronic states are necessary to fully leverage the capabilities of CsPbBr 3 crystals in practical high-energy radiation detection systems.

Bridgman↗
DOE OSTI2022

Cesium lead bromide semiconductor radiation detectors: crystal growth, detector performance and polarization

Cesium lead bromide (CsPbBr 3 ) is an upcoming semiconductor radiation detector that has the potential to match the detection properties of cadmium zinc telluride (CZT) and thallium bromide (TlBr). In this paper, we report on CsPbBr 3 gamma detectors with an uncorrected energy resolution of 2% at 662 keV with photopeak-to-Compton ratios as high as 14.3 and hole mobility-lifetime products (μτ h ) as high as 1.7 × 10 –2 cm 2 V –1 . Furthermore, we demonstrate that the processes employed for material purification and crystal growth of high-performing devices are scalable, and large (up to 65 mm in diameter) ultrahigh purity CsPbBr 3 crystals have been successfully grown. Furthermore by using optimized growth conditions and detector fabrication processes, we were able to mitigate the polarization problem where it was revealed that the polarization process is highly dependent on the crystal quality and the electric field direction with respect to the orientation of the crystal.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2022

Predicted performance of a tangential viewing hard x-ray camera for the DIII-D high field side lower hybrid current drive experiment

High field side launch of lower hybrid current drive (LHCD) has improved accessibility and penetration over low field side launch on DIII-D. Simulations predict single pass absorption under a wide range of plasma conditions. Hard x-ray (HXR) measurement of LHCD generated fast electron bremsstrahlung (50–250 keV) will validate wave propagation and absorption. Emissivity profiles are recovered from one-dimensional inversion of HXR brightness to determine LH damping location, fast electron slowing down time, and some indication of the fast electron energy. The camera will be implemented by populating 32 tangential sightlines of the existing Gamma Ray Imager with Kromek SPEARTM Cadmium Zinc Telluride (CZT) detectors sensitive to 10–1000 keV photons with 10 keV energy resolution. Expected count rates allow for <0.5 ms time resolution. Pulses are processed using 50 ns shaping time Cremat CR-200 Gaussian shaping modules and are digitized by 25 MHz D-TACQ ACQ216 digitizers. The performance of the HXR camera is evaluated by comparing predicted fast electron density profiles and inverted synthetic brightnesses obtained from the ray-tracing/Fokker–Planck codes GENRAY/CQL3D. Inversions closely matched predicted fast electron profiles for a range of experimental parameters.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Multi-channel front-end ASIC for a 3D position-sensitive detector

Arrays of 3D position-sensitive detectors (3DPSD), operating at room temperature and using cadmium zinc telluride (CZT) and thallium bromide (TIBr) sensors, are suitable for gamma-ray spectrometry in many applications. One detector configuration, the 3D position-sensitive Virtual Frisch-Grid detector (VFG), is particularly advantageous for integrating into large area arrays. The signals generated inside each detector of the array are captured with the anode, cathode and four pads that enable the reconstruction of the position and energy of the ionizing interaction by measurements of amplitude and timing of the signals. For these applications, a low-noise front-end ASIC has been developed, capable of processing bipolar signals (needed because of AC-coupling of certain electrodes). The ASIC can be coupled to an ADC in order to form a compound “waveform digitizer” capable of post-processing the analog signals and determining amplitude and timing information. This paper describes a 32-channel front-end ASIC that is suitable for reading out a 3 × 3 or 4 × 4 element matrix in the VFG configuration. Each channel is composed of a low-noise charge amplifier with an adaptive continuous reset feedback circuit suitable for both positive and negative charge, a first order shaper and a single-to-differential converter output stage. Voltage and current references are all internally generated by 10-bit DACs and the chip is fully controllable with the I 2 C communication protocol. The readout channel response has been verified using the implemented injection circuit. Linear behavior up to ~75 ke ± with the gain of ~80 mV/fC, and up to ~200 ke ± with the gain of ~30 mV/fC was demonstrated. In conclusion, the first test result waveforms using a 137 Cs radioactive source on a 5 × 5 × 12 mm 3 TIBr crystal are reported.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Improving CdMnTe Detector Performance by Adding 2% of Selenium

About 2% of selenium was added to CdMnTe (CMT) to reveal the role of selenium in CMT material used as a gamma-ray detector. The average etch-pit density (EPD) in a typical 2-in CdMnTeSe (CMTS) wafer was measured to be about 8.3×10 3 cm –2 except for the edge regions, and the radial nonuniformity of the bandgap along the wafer was about 2-meV. The typical mobility-lifetime product of electrons and holes was evaluated to be 3.06×10 –3 cm 2 /V and 3.1×10 –4 cm 2 /V, respectively. The energy resolution of the 122-keV photo-peak for a Co-57 radioactive source with a planar CMTS detector was 5.2%, demonstrating a positive effect associated with adding dilute amounts of Se to CMT. Finally, the enhanced detector performance in a planar CMTS detector is attributed to an improved value of hole mobility-lifetime product in CMTS, which mitigates the adverse hole tailing effect found in CdZnTe (CZT) and CMT detectors.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

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↗
DOE OSTI2024

Radiation Monitoring for Volatilized Zinc Contamination Using Gamma-Ray Imaging and Spectroscopy

Gamma-ray imaging is a tool that has grown in importance in the applications of non-destructive assay (NDA) for radioactive survey and analysis of nuclear facilities. Imaging techniques have shown great promise in providing valuable information involving radioactive waste management and contamination prevention. For the application studied in this work, 65 Zn has been identified as a radioactive contaminant during tritium extraction. Due to the volatile nature of 65 Zn under the pressure and temperature changes during extraction operations, 65 Zn can easily travel through components of the extraction system as vapor, making it difficult to trap. Previous research involving the development of a filtration system showed that the 65 Zn can be trapped, mitigating product contamination. However, during the extraction process, direct analysis of the equipment to confirm that zinc contamination is trapped in the filter and has not spread to other components is impractical. Here, in this situation, the need to assay the location of the contamination with little-to-no interference with operations is vital. In this work, we demonstrate the use of a commercialized 3D position-sensitive CdZnTe (CZT) gamma-ray imaging spectrometer to provide analysis of the 65 Zn contamination. Onsite measurements during an extraction process are studied to assess the location and migration of the 65 Zn. The results obtained from real-time glovebox monitoring demonstrate the feasibility of gamma-ray imaging for localizing the contamination and providing a preliminary qualitative assessment that is intended to be used in future work quantifying the contamination build-up and activity over time.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Spectral Peak Enhancement by Combining Trusted Response Elements via Machine Learning (SPECTRE-ML) v0.8.0

SPECTRE-ML (Spectral Peak Enhancement by Combining Trusted Response Elements via Machine Learning) is a machine learning based program for finding optimal clusters of radiation detector segments (i.e., pixels or voxels) in order to improve spectral performance. It provides facilities for pre-processing and analyzing training datasets, running ML algorithms, and evaluating and visualizing outputs. SPECTRE-ML outperforms simpler ad-hoc segmentation methods such as uniform depth clusters, learning detector performance trends such as dead layers, edge effects, and gain shifts. Although extensible to arbitrary highly-segmented spectroscopic radiation detectors, SPECTRE-ML currently focuses on improving spectral performance in highly-segmented CdZnTe (CZT) detectors for International Atomic Energy Agency (IAEA) non-destructive assay (NDA) safeguards tasks.

Vavrek, Jayson↗
DOE OSTI2023

Quantum Dot Based Solid-State Radiation Detectors

The detection and accurate identification of nuclear material is critical to the advancement of national security, medical technology, and environmental prosperity. The gold standard solid-state detector HPGe, suffers from high manufacturing costs and the need to operate at cryogenic temperatures to ensure reliable energy resolution. The other most common solid-state detector, cadmium zinc telluride (CZT), has the ability to operate at room temperature, but the grow process results in impurities decreasing performance. In this paper we have developed a continuous flow synthesis able to mass produce targeted size cadmium selenide quantum dots. The implementation of these QDs in QD/MEH-PPV composites has the ability to rival HPGe energy resolution at room temperature.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Evaluation of the Stability of Edge-Passivated CZTS Radiation Detectors

CdZnTeSe (CZTS) is a next gen replacement room temperature radiation detector that solves common issues with modern CZT detectors. • Surface states can trap radiation induced carriers and can act as leakage current pathways requiring detectors to passivated for optimal performance. • In this work, we seek to identify the best passivation technique for CZTS detectors.

KLEPPINGER, JOSHUA↗
DOE OSTI2024

Synchrotron-based Characterization Techniques for Radiation Detection Materials and Devices: An Overview

High-performance room-temperature radiation detectors (high energy resolution for spectrometers, high spatial resolution for imaging devices, and low defect-density for high flux applications) are needed for photon energies (>20 keV) that are not well suited for silicon detectors. Applications for such radiation detectors include nonproliferation, synchrotron, medical, astrophysics, and homeland security. Material- and device- characterization to understand and solve the limiting factors of radiation detection materials and devices is a core element of a radiation detector development R&D program. This presentation will give an overview on the two main synchrotron-based characterization techniques that have been employed by the authors in the last ~20 years: (1) White Beam X-ray Diffraction Topography and (2) Micron-scale detector mapping. A perfect (one domain) crystal (radiation detection material) is a requirement to achieve a highperformance radiation detector. White Beam X-ray Diffraction Topography (WBXDT) allows the rapid screening of the crystallinity of the detector material. With WBXDT we can quickly screen CZT and other crystals to make sure they have only one domain, and to see the presence of extended defects and strain fields.

Camarda, Giuseppe S.↗
DOE OSTI2025

Detector Performance on Surface Passivation and its Long-Term Stability

Surface passivation is an ideal technique to prepare the surfaces of fabrication Cadmium Zinc Telluride (CZT) and related semiconductor devices such as Cadmium Zinc Tellurium Selenide (CZTS). Surface passivation techniques reduce the effects of aging in the detector [1]. Surface performance effects on material performance can result in fluctuations in energy resolution over time (such as periods of a year or more). The long-term stability of surface passivation with Potassium Hydroxide (KOH) was observed with measurement of 1) current (nano Amp) vs voltage (V) and 2) spectral response and energy resolution throughout the years. Three CZTS detector samples of M2, M3, and M4 were examined using a photomultiplier tube and voltage amplifier. The Bridgman technique is used to grow the CZTS used in this study.

Johnson, Kirsten [Morgan State Univ., Baltimore, M↗
DOE OSTI2025

Gamma and Neutron Measurement and Modeling of Irradiated TRISO Fuel

Given the unique characteristics of the PBR fuel cycle, both gamma and neutron measurements are expected to play important roles in performing and maintaining nuclear material control and accounting for spent pebbles to safeguard the fuel cycle. Given the lack of irradiated pebbles in the US, a variety of irradiated TRISO fuel samples with wide ranges of burnups and cooling times available at ORNL were used in this work. A large number of gamma and neutron measurements have been performed on these samples to collect data to test the various detectors and to benchmark the computer models to simulate the depletion and decay of the fuel and the measurements themselves. Two neutron detectors, including a custom-made detector and the Very High-Performance Neutron Multiplicity Counting, were used to measure the neutrons emitted by these TRISO samples. Three gamma spectrometry detectors, including an HPGe and the M400 CZT detector, were used to measure gamma-ray emissions from these samples. The M400 was recently adopted by the IAEA for fresh uranium measurements, but it was tested for spent fuel measurements prior to this project. Detailed MCNP models were developed to simulate these neutron and gamma measurements. Some GADRAS models were also developed to cross check the MCNP models for the gamma measurements. It was found challenging to perform neutron measurements in the hot cell due to the high background counts. Close agreements were observed between the simulated and measured neutron count rates in both detectors’ measurements of californium calibration sources. Both the HPGe and M400 detectors were able to measure the 604 and 662 keV peaks from these samples, which are the two most important peaks used to infer fuel burnup. Although the M400 detector did not have nearly good energy resolution and did not detect some of the minor peaks as the HPGe detector, it was found to be capable of handling significantly higher dose rates than HPGe. Given the complexities in the TRISO samples (e.g., different samples sizes) and uncertainties in the alignments between the detector and the TRISO fuel inside the containers, large scatters were found between the peak area rates and the samples’ burnups. However, the 604/662 peak ratios were found to trend well with the samples’ burnups among most samples in both measured and simulated results.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

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↗
DOE OSTI2022

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↗