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At least 199 records · Page 11

Uranium Holdup Monitoring with Compton Imaging as Function of Depth and Mass

Material Control and Accountability (MC&A) programs track masses of materials flowing through production processes, where some material remains in process equipment as holdup. Quantification of these masses using gamma emissions typically involves usage of a well characterized radiation detector and assumptions of geometric configuration to constrain detection efficiencies, where the Generalized Geometry Holdup (GGH) method is often used. Uncertainties on the order of ±50% are observed, where the difficulties arise based on the asymmetric and gradient distributions of material that do not fall within the bounds of GGH. Gamma imagers provide a possible means to improve this geometric knowledge. This work describes the process used in creating a series of mass standards to aid the development of imaging algorithms for quantification.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Contributions to the BeEST sterile neutrino search

Sterile neutrinos are hypothetical right-handed leptons that have been postulated as extensions to the Standard Model to help explain the origin of neutrino masses and the matter-antimatter asymmetry in the Universe. Sterile neutrinos with keV-scale masses are also a promising candidate for dark matter. LLNL and the Colorado School of Mines are developing an experiment to search for sterile neutrinos by measuring the \Beryllium-7 Electron capture in Superconducting Tunnel junctions (STJs)" (the \BeEST" Experiment). When 7 Be implanted into STJ radiation detectors decays by electron capture, the neutrino escapes and the energy of the recoiling 7 Li nucleus can be measured with high accuracy. Using conservation of energy and momentum, the mass of the emitted neutrino can then be found. Sterile keV neutrinos would generate additional peaks in the spectrum, and the experiment uses high-resolution STJs to observe such a potential signal. During my internship, I contributed to different aspects of the BeEST experiment. I designed a UHV setup for X-ray spectroscopy analysis with STJs. It will allow high-resolution X-ray spectroscopy of different materials to examine the broadening in the BeEST spectra, the origins of which are unknown but may be related to material effects inside the STJ detectors. The design accounts for the specific demands of the BeEST project, but provides a degree of flexibility that makes it useful for other potential STJ projects. Additionally, to test the accuracy of the electronics and data analysis routine, an arbitrary waveform generator (AWG) will be used to generate simulated spectra that contain sterile neutrino signals of a specified mass and admixture. For this I programmed an AWG to output random STJ signals whose amplitudes follow the appropriate user-de ned probability distribution. The AWG signals can be input into the 32-channel preamplifier to simulate any spectrum of interest and test the uniformity of the amplifier chain, as well as the sensitivity of the data analysis.

42 ENGINEERING↗

Sensor Placement Optimization Study for the Built Environment: Operational Use Cases

Systems of fixed-position radiation sensors can provide information that assists emergency responders following nuclear and radiological incidents. State, local, tribal, and territorial (SLTT) government agencies that implement systems of fixed-position sensors are faced with numerous decisions regarding sensor selection, quantity, and placement. To develop guidance on implementation of radiation detection systems, we simulated the release of radioactive material in an urban environment using a combination of three models: the Weather Research Forecasting (WRF), Quick Urban and Industrial Complex (QUIC), and Monte Carlo N-Particle (MCNP) models. We then evaluated the performance of several hypothetical sensor systems. The small number of simulations we conducted are not sufficient to generate definitive design guidance for radiation sensor systems, but we did identify trends that would be of interest to emergency planners. For a scenario that releases 1000 curies of Cs-137, radiation detectors were needed at 500-meter intervals to have a high likelihood of event detection and to estimate source location and plume detection. We also noted that optimal detector altitude varied with distance to the source. We recommend additional research in this area be conducted to support developing sensor placement guidelines that expand on a range of locations, isotopes, activity levels, and different weather conditions. Original simulation strategies included a range of environments, additional radioisotopes (Am241 and AmBe), and a larger selection of sensor types. These types of expansions would support SLTT guidance on sensor system recommendations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Matrix-Assisted Ionization of Molecular Uranium Species

Matrix-assisted ionization (MAI) demonstrates high sensitivity for a variety of organic compounds; however, few studies have reported the application of MAI for the detection and characterization of inorganic analytes. Trace-level uranium analysis is important in the realms of nuclear forensics, nuclear safeguards, and environmental monitoring. Traditional mass spectrometry methods employed in these fields require combinations of extensive laboratory chemistry sample preparation and destructive ionization methods. There has been recent interest in exploring ambient mass spectrometry methods that enable timely sample analysis and higher sensitivity than what is attainable by field-portable radiation detectors. Rapid characterization of uranium at nanogram levels is demonstrated in this study using MAI techniques. Mass spectra were collected on an atmospheric pressure mass spectrometer for solutions of uranyl nitrate, uranyl chloride, uranyl acetate, and uranyl oxalate utilizing 3-nibrobenzonitrile as the ionization matrix. The uranyl complexes investigated were detectable, and the chemical speciation was preserved. Sample analysis was accomplished in a matter of seconds, and limits of detection of 5 ng of uranyl nitrate, 10 ng of uranyl oxalate, 100 ng of uranyl chloride, and 200 ng of uranyl acetate were achieved. The observed gas-phase speciation was similar to negative-ion electrospray ionization of uranyl compounds with notable differences. Six matrix-derived ions were detected in all negative-ion mass spectra, and some of these ions formed adducts with the uranyl analyte. Subsequent analysis of the matrix suggests that these molecules are not matrix contaminants and are instead created during the ionization process.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

$β$-delayed-neutron studies of 135,136 Sb and 140 I performed with trapped ions

In this work, Beta-delayed-neutron $(βn)$ spectroscopy was performed using the Beta-decay Paul Trap and an array of radiation detectors. The $βn$ branching ratios and energy spectra for 135,136 Sb and 140 I were obtained by measuring the time of flight of recoil ions emerging from the trapped ion cloud. These nuclei are located at the edge of an isotopic region identified as having $βn$ branching ratios that impact the $r$-process abundance pattern around the A ≈ 130 peak. For 135,136 Sb and 140 I, $βn$ branching ratios of 14.6(13)%, 17.6(29)%, and 7.6(28)% were determined, respectively. The $βn$ energy spectra obtained for 135 Sb and 140 I are compared with results from direct neutron measurements, and the $βn$ energy spectrum for 136 Sb has been measured for the first time.

42 ENGINEERING↗

Study on Application of Distributed Network of Sensors with List Mode for NMAC Literature Review

Nuclear material accounting and control (NMAC) for nuclear security detects, deters, and resolves questions related to unauthorized removal (i.e. theft) or misuse of nuclear material. NMAC also serves as a key insider threat mitigation measure and aids in recovery of nuclear material that is missing. Effective nuclear security depends on NMAC for timely and accurate information about nuclear material types, quantities, and locations. Bulk nuclear material processing facilities, however, present unique challenges for effective NMAC due to the presence of large quantities of material in-process and the accumulation of residual material holdup within process equipment. These holdup accumulations can obscure accurate physical inventory taking and complicate efforts to resolve NMAC irregularities at the facility level. Bulk material monitoring systems often rely on material balance calculations and indirect measurement techniques, which may mask protracted theft of smaller amounts of nuclear material. These monitoring limitations have generated increased interest in continuous monitoring technologies, including distributed non-destructive assay (NDA) sensor networks capable of providing real-time or near-real-time measurement of material movement and accumulation within bulk processing environments. Recent advancements in distributed networks of NDA radiation detectors and sensing technologies provide an opportunity to address these limitations. Although such distributed sensor networks have been implemented in select facilities for IAEA Safeguards applications, their potential for supporting NMAC functions specifically tailored to nuclear security objectives remains largely unexplored. Furthermore, emerging list-mode data acquisition technologies have reached high technology readiness levels, enabling time-correlated detection of nuclear events across multiple temporal scales. These capabilities provide enhanced opportunities for accurate holdup measurement, continuous process monitoring, and improved detection of material theft or misuse over time. The increasing global expansion of civil nuclear power and development of related bulk material processing facilities, including those supporting high-assay low-enriched uranium (HALEU) and other advanced reactor fuel fabrication, further increases the need for advanced measurement and monitoring strategies for NMAC.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Enhanced sensitivity to trace 238 U impurity of sapphire via coincidence neutron activation analysis

Sapphire has mechanical and electrical properties that are advantageous for the construction of internal components of radiation detectors such as time projection chambers and bolometers. However, it has proved difficult to assess its 232 Th and 238 U content down to the picogram per gram level. Here, this work reports an experimental verification of a computational study that demonstrates 𝛾⁢𝛾 coincidence counting, coupled with neutron activation analysis (NAA), can reach ppt sensitivities. Combining results from 𝛾⁢𝛾 coincidence counting with those of earlier single-𝛾 counting based NAA shows that a sample of Saint Gobain sapphire has 232 Th and 238 U concentrations of <0.26 ppt and <2.3 ppt, respectively; the best constraints on the radiopurity of sapphire.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Enhanced Neutron and γ-Ray Detection via 6 Li Substitution in Undoped and Tl-Doped Zero-Dimensional Perovskite Cs 3 Cu 2 I 5 Scintillators

Radiation detectors are crucial in a wide variety of research and commercial applications, such as oil and gas exploration, medical imaging, nuclear nonproliferation, and homeland security. Neutron and gamma-ray detectors are fundamental components in portal monitors at ports and border crossings, bolstering national security against radiological threats. This study presents a dual-mode scintillator, undoped and Tl-doped 6 Li-Cs 3 Cu 2 I 5 , and demonstrates its potential as a promising material for simultaneous thermal neutron and gamma-ray detection. We explore the Bridgman growth of both undoped and thallium doped Li → Cu and Li → Cs substitutional systems with various Li doping levels and assess their impact on scintillation properties. Under 662 keV gamma-ray excitation, the undoped crystals had light yields up to 35,900 ph/MeV, with energy resolutions down to 4.5%. The Tl-doped crystals performed better than the undoped crystals with light yields peaking at 65,900 ph/MeV and energy resolutions as low as 3.5%. When exposed to a moderated 252 Cf excitation source, our crystals had light yields between 102,900 and 167,200 photons per thermal neutron capture, with a full energy thermal neutron peak reaching 3 MeV in gamma equivalent energy. Pulse shape discrimination studies reveal well-separated gamma and neutron events, resulting in Figure-Of-Merit (FOM) as high as 3.7. Furthermore, these findings highlight the potential of Li-doped Cs 3 Cu 2 I 5 as a viable candidate for next-generation dual-mode scintillators.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Investigation of the Solution Chemistry of Hybrid Organic–Inorganic Indium Halides for New Material Discovery

Recently, metal halide perovskites (MHPs) have emerged as a new class of materials for optical and electronic applications such as solar cells and ionizing radiation detectors. Although the solution-processability of MHPs is among their greatest advantages, the solution chemistries of most metal halide systems and their relationship with the observed structural and chemical diversity are poorly understood. In this work, we study the solution chemistry of a model indium halide system, methylammonium (MA)–In–Br, using a combination of the UV–vis spectroscopy, electrospray ionization mass spectrometry (ESI-MS) measurements, small-angle X-ray scattering (SAXS), and density functional theory (DFT) calculations. Our results show that indium could form either octahedral [InBr 6 3– ] or tetrahedral [InBr 4 – ] anions in solution or a combination of both, depending on the loading ratios of MABr and InBr 3 reactants. Understanding the solution chemistry of this system and recognizing the optical fingerprints of these polyanions allow for targeted crystallization of two novel compounds: MAInBr 4 featuring tetrahedral [InBr 4 – ] anions and MA 2 InBr 5 containing both octahedral [InBr 6 3– ] and tetrahedral [InBr 4 – ] anions. Further increase of the MABr content leads to the formation of previously reported MA 4 InBr 7 , containing only octahedral [InBr 6 3– ] anions separated by Br – anions. Furthermore, our results suggest that understanding the solution chemistry of multinary metal halide systems could be a valuable tool for discovering functional materials for practical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effects of Selenium Doping in Zinc Telluride from First Principles

We report point defects and compensation in zinc telluride have been subjects of study for several decades due to the compound’s scientific/technological applications. Despite this, there remains some disagreement in the literature as to the fine details of its defect chemistry. Recently, it has also come under renewed interest due to the emerging Cd( 1–x )Zn x Te( 1–y )Se y material family, used in nuclear radiation detector applications. In this article, we use state-of-the-art computational tools to re-examine the native defect chemistry of ZnTe and explore how it changes upon addition of selenium using density functional theory with screened hybrid exchange–correlation functionals, thermochemical models of the equilibration environment, and statistical mechanics models of the point defect ensemble.

II-VI semiconductors↗

Coloring Tetrahedral Semiconductors: Synthesis and Photoluminescence Enhancement of Ternary II-III 2 -VI 4 Colloidal Nanocrystals

Ternary tetrahedral II-III 2 -VI 4 semiconductors, where II is Zn or Cd, III In or Ga, and VI S, Se, or Te, are of interest in UV radiation detectors in medicine and space physics as well as CO 2 photoreduction under visible light. We synthesize colloidal II-III 2 -VI 4 semiconductor nanocrystals from readily available precursors and ascertain their ternary nature by structural and spectroscopic methods, including 77 Se solid-state NMR spectroscopy. The pyramidally shaped nanocrystals range between 2 and 12 nm and exhibit optical gaps of 2–3.9 eV. In the presence of excess anions on the particle surface, treatment with Lewis acidic, Z-type ligands results in better passivation and enhanced photoluminescence. Electronic structure calculations reveal the most stable, lowest energy polymorphs and coloring patterns. This work will pave the way toward more environmentally friendly, ternary semiconductors for optoelectronics and electrocatalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

New Ultrafast Scintillators with Core Valence Luminescence: Cs 2 MgCl 4 and Cs 3 MgCl 5

Future experiments in high energy physics and medical imaging require radiation detectors having properties which are not presently available. The main limitations arise from lack of suitable scintillation crystals. This dilemma prompts the need for research leading to the discovery of new fast and bright scintillator materials that combine unique properties to fulfil modern experiment requirements without compromises. In this work, single crystals of Cs 2 MgCl 4 and Cs 3 MgCl 5 up to 12 mm in diameter are grown via the vertical Bridgman method. Scintillation properties are reported for the first time, and core valence luminescence is observed for both compounds. X-ray excited radioluminescence emission of Cs 2 MgCl 4 is centered at 295 nm, with a scintillation decay time of 2.25 ± 0.05 ns and relatively high core-valence light yield of 2,200 ± 110 ph/MeV. Cs 3 MgCl 5 has two main emission peaks centered at 242 nm and 302 nm, decay time of 1.46 ± 0.05 ns, and light yield of 1,340 ± 70 ph/MeV. The better coincidence time resolution (CTR) is obtained with Cs 2 MgCl 4 , which is measured to be 129 ± 4 ps FWHM. Density functional theory (DFT) calculations are also performed and provide supporting evidence that the observed scintillation originates from core valence luminescence. Furthermore, the combination of speed and brightness of these new scintillators could be useful for fast timing applications in which moderately dense materials are required.

36 MATERIALS SCIENCE↗

Waveform processing using neural network algorithms on the front-end electronics

In a multi-channel radiation detector readout system, waveform sampling, digitization, and raw data transmission to the data acquisition system constitute a conventional processing chain. The deposited energy on the sensor is estimated by extracting peak amplitudes, area under pulse envelopes from the raw data, and starting times of signals or time of arrivals. However, such quantities can be estimated using machine learning algorithms on the front-end Application-Specific Integrated Circuits (ASICs), often termed as “edge computing”. Edge computation offers enormous benefits, especially when the analytical forms are not fully known or the registered waveform suffers from noise and imperfections of practical implementations. In this work, we aim to predict peak amplitude from a single waveform snippet whose rising and falling edges containing only 3 to 4 samples. We thoroughly studied two well-accepted neural network algorithms, Multi-Layer Perceptron (MLP) and Convolutional Neural Network (CNN) by varying their model sizes. Further, to better fit front-end electronics, neural network model reduction techniques, such as network pruning methods and variable-bit quantization approaches, were also studied. By combining pruning and quantization, our best performing model has the size of 1.5 KB, reduced from 16.6 KB of its full model counterpart. It can reach mean absolute error of 0.034 comparing to that of a naive baseline of 0.135. Such parameter-efficient and predictive neural network models established feasibility and practicality of their deployment on front-end ASICs.

47 OTHER INSTRUMENTATION↗

Exploration of Neutron-Rich Isotopes around N = 50 via the In-Flight Fission of a 345 MeV/Nucleon 238 U Beam

A search for new neutron-rich isotopes beyond $Z=28$ and $N=50$ was performed using a 345 MeV/nucleon $^{238}$U beam at RI Beam Factory in RIKEN Nishina Center. The BigRIPS separator and state-of-the-art radiation detectors were used to efficiently separate and identify the produced nuclei. For the first time, we have observed and determined the production cross sections for eight neutron-rich isotopes $^{72}$Cr, $^{74,75}$Mn, $^{77}$Fe, $^{79,80}$Co, $^{85}$Cu, and $^{90}$Ga. This study broadens our understanding of nuclear existence and paves the way for investigating the properties of neutron-rich medium-mass nuclei.

Shimizu, Yohei [RIKEN, Saitama (Japan); et al.]↗

First study of the $^{139}\text{Ba}(n,y)^{140}\text{Ba}$ reaction to constrain the conditions for the astrophysical $\mathcal{i}$ process

New astronomical observations point to a nucleosynthesis picture that goes beyond what was accepted until recently. The intermediate “i” process was proposed as a plausible scenario to explain some of the unusual abundance patterns observed in metal-poor stars. The most important nuclear physics properties entering i-process calculations are the neutron-capture cross sections and they are almost exclusively not known experimentally. In this report we provide the first experimental constraints on the 139 Ba(n,γ) 140 Ba reaction rate, which is the dominant source of uncertainty for the production of lanthanum, a key indicator of i-process conditions. This is an important step towards identifying the exact astrophysical site of stars carrying the i-process signature.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Ultrahigh supercurrent density in a two-dimensional topological material

Ongoing advances in superconductors continue to revolutionize technology thanks to the increasingly versatile and robust availability of lossless supercurrents. In particular, high supercurrent density can lead to more efficient and compact power transmission lines, high-field magnets, as well as high-performance nanoscale radiation detectors and superconducting spintronics. In this work, we report the discovery of an unprecedentedly high superconducting critical current density (17 MA / cm 2 at 0 T and 7 MA / cm 2 at 8 T) in 1T'–WS 2 , exceeding those of all reported two-dimensional superconductors to date. 1T'–WS 2 features a strongly anisotropic (both in- and out-of-plane) superconducting state that violates the Pauli paramagnetic limit signaling the presence of unconventional superconductivity. Spectroscopic imaging of the vortices further substantiates the anisotropic nature of the superconducting state. More intriguingly, the normal state of 1T'–WS 2 carries topological properties. The band structure obtained via angle-resolved photoemission spectroscopy and first-principles calculations points to a Z 2 topological invariant. The concomitance of topology and superconductivity in 1T'–WS 2 establishes it as a topological superconductor candidate, which is promising for the development of quantum computing technology.

36 MATERIALS SCIENCE↗

Point defects in CdTe and CdSeTe alloy: a first principles investigation with DFT+U

CdTe and its alloy CdSeTe are widely used in optoelectronic devices, such as radiation detectors and solar cells, due to their superior electrical properties. However, the formation of defects and defect complexes in these materials can significantly affect their performance. As a result, understanding the defect formation and recombination processes in CdTe and CdSeTe alloy is of great importance. In recent years, density functional theory (DFT) calculations have emerged as a powerful tool for investigating the properties of defects in semiconductors. In this paper, we use DFT+U calculations to comprehensively study the properties of intrinsic defects as well as extrinsic defects induced by commonly used dopants, such as Cu and group V elements, in CdTe and CdSeTe alloy. This work provides insights into the effects of these defects on the electrical and optical properties of the material.

14 SOLAR ENERGY↗

Investigation of Timing Properties for an Event Driven with Access and Reset Decoder Readout Architecture for a Pixel Array

The large number of data generating sources (data channels) on a single chip requires appropriate techniques to manage a readout from these channels. One of the main methods is sharing a medium of transmission, which requires arbitration to avoid collisions or deadlocks. Existing solutions face several problems such as a dead time, unintended prioritization or metastability. That is why we decided to create a new readout architecture named EDWARD i.e., Event Driven with Access and Reset Decoder. The EDWARD architecture gets rid of the earlier mentioned problems and mitigates the other ones. However, due to the use of logic circuits outside a standard cell library, which are hard to characterize, we were challenged to perform an additional transient analysis to validate the architecture. Here we show a methodology and the results of the simulations. Based on the results obtained we can confirm the functional correctness of the system and plan the optimization of operating conditions in order to achieve better performance. Our goal is to use the EDWARD architecture in the future radiation detectors to be built at Brookhaven National Laboratory.

47 OTHER INSTRUMENTATION↗