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At least 289 records · Page 16

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.↗

Stereoscopic detection of hot spots in superfluid 4 He (He II) for accelerator-cavity diagnosis

Superconducting radio-frequency (SRF) cavities cooled by superfluid 4He (He II) are building blocks of many modern particle accelerators due to their high quality factor. However, Joule heating from sub-millimeter surface defects on cavities can lead to cavity quenching, which limits the maximum acceleration gradient of the accelerators. Developing a non-contacting detection technology to accurately locate these surface hot spots is the key to improve the performance of SRF cavities and hence the accelerators. In a recent proof-of-concept experiment, we demonstrated that a molecular tagging velocimetry (MTV) technique based on the tracking of a He molecular tracer line created nearby a surface hot spot in He II can be utilized to locate the hot spot. In order to make this technique practically useful, here we describe our further development of a stereoscopic MTV setup for tracking the tracer line’s motion in three-dimensional (3D) space. We simulate a quench spot by applying a transient voltage pulse to a small heater mounted on a substrate plate. Images of the drifted tracer line, taken with two cameras from orthogonal directions, are used to reconstruct the line profile in 3D space. Here, a new algorithm for analyzing the 3D line profile is developed, which incorporates the finite size effect of the heater. We show that the center location of the heater can be reproduced on the substrate surface with an uncertainty of only a few hundred microns, thereby proving the practicability of this method.

43 PARTICLE ACCELERATORS↗

Probing and controlling oxygen impurity diffusion in h -BN semi-bulk crystals

Combining its unique features of ultrawide bandgap (UWBG) and two-dimensional nature, h-BN has been explored for emerging applications such as deep ultraviolet optoelectronic devices and single photon emitters. One of the unusual applications of h-BN is for solid-state neutron detectors by utilizing the property of high thermal neutron capture cross section of B-10 as well as its UWBG properties. Although a record high detection efficiency of 59% has been attained by h-BN detectors, the understanding/minimization of defects and impurities is still needed to further advance the h-BN material and detector technologies. We report metal organic chemical vapor deposition growth and oxygen (O) impurity diffusion in thick h-BN. The diffusion coefficient (D) of O impurities has been measured via the evolution of an oxygen related emission with the etching depth, providing a value of D of ∼ 2 × 10−13 cm2/s at 1450 °C and supporting the interpretation that oxygen in h-BN is a substitutional donor. A multiple-buffer-layer approach was employed to mitigate to a certain degree the issue of oxygen diffusion from sapphire substrate during growth. It was demonstrated that the performance of h-BN neutron detectors fabricated from the wafer incorporating multiple buffer layers was significantly improved, as manifested by the enhanced thermal neutron detection efficiency. The advancement of the crystal growth technology of h-BN semi-bulk crystals creates applications in optoelectronic and power electronic devices utilizing the UWBG semiconductor properties of h-BN, while high efficiency h-BN neutron detectors have the potential to supplant the traditional He-3 gas detectors in various application areas by offering the obvious advantages of UWBG semiconductor technologies.

Physics↗

Combining In-situ Diagnostics and Data Analytics for Discovery of Process-Structure-Property Relationships in AM parts – A Step Toward Digital Twins

In-situ additive manufacturing (AM) diagnostic tools (e.g., optical/infrared imaging, acoustic, etc.) already exist to correlate process anomalies to printed part defects. This current work aimed to augment existing capabilities by: 1) Incorporating in-situ imaging w/ machine learning (ML) image processing software (ORNL- developed "Peregrine") for AM process anomaly detection 2) Synchronizing multiple in-situ sensors for simultaneous analysis of AM build events 3) Correlating in-situ AM process data, generated part defects and part mechanical properties The key R&D question investigated was to determine if these new combined hardware/software tools could be used to successfully quantify defect distributions for parts build via SNL laser powder bed fusion (LPBF) machines, aiming to better understand data-driven process-structure-property- performance relationships. High resolution optical cameras and acoustic microphones were successfully integrated in two LPBF machines and linked to the Peregrine ML software. The software was successfully calibrated on both machines and used to image hundreds of layers of multiple builds to train the ML software in identifying printed part vs powder. The software's validation accuracy to identify this aspect increased from 56% to 98.8% over three builds. Lighting conditions inside the chamber were found to significantly impact ML algorithm predictions from in-situ sensors, so these were tailored to each machine's internal framework. Finally, 3D part reconstructions were successfully generated for a build from the compressed stack of layer-wise images. Resolution differences nearest and furthest from the optical camera were discussed. Future work aims to improve optical resolution, increase process anomalies identified, and integrate more sensor modalities.

36 MATERIALS SCIENCE↗

Defect-induced formation and frustration-driven multiple magnetic transitions in Gd 2 Co 0.90 Si 2.90

A new ternary compound, Gd 2 Co 0.90 Si 2.90 , has been synthesized in a chemically single phase by deliberately introducing lattice vacancies in the Co and Si sites. The system is characterized by DC magnetization, heat capacity, resistivity and density functional theory (DFT) calculations. Here, a detailed experimental study reveals that the system exhibits an antiferromagnetic transition below T N = 11.3 K followed by spin freezing behaviour below T B ~ 4.8 K. An additional high-temperature magnetic transition could also be detected at T H ~ 150 K, which is short range in character and is associated with defect-induced polarization of the conduction electrons. The spin-glass-like state formation in the system is additionally bolstered by the observation of magnetic relaxation and associated aging phenomena as well as the magnetic memory effect. On the basis of non-equilibrium dynamical behaviour, we argue that the glassy state in this compound favours the hierarchical model over the droplet model. DFT calculations and experimental outcomes establish that the ground state is magnetically frustrated due to the small energy difference between distinct spin configurations having closely spaced ground-state energies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The promise of optical NMR spectroscopy for experimental aqueous geochemistry

Here, we discuss new quantum technologies being adapted to detect extraordinarily small magnetic fields. The signals are derived from the stimulated emission of light from single-atom defects in diamonds. The intensity of light reports the spin state of the electrons in the color center. The physics is relevant to geochemists because it points to a means of conducting NMR experiments on solutions in diamond-anvil cells. Because the method is so sensitive, it can detect signals in subnanoliter volumes, making work at elevated temperatures and pressures possible, and also on solutions that are dangerous in larger volumes.

58 GEOSCIENCES↗

Performance Study of Virtual Frisch Grid CdZnTeSe Detectors

Nuclear detectors for x-ray and gamma-ray spectroscopy and imaging are a vital tool in many homeland security, medical imaging, astrophysics and other applications. Most of these applications require room-temperature operation due to the operational constraints imposed by a cryogenic cooling system. CdZnTe (CZT) has been the main material with the desired detection properties, and CZT crystals have been used commercially for three decades. However, CdZnTe still suffers from long-standing issues of high densities of performance-limiting intrinsic defects such as Te inclusions and networks of dislocation walls (sub-grain boundaries). A recently invented new quaternary material CdZnTeSe showed excellent material properties for radiation detection. The material was found to be free from dislocation networks, possess reduced Te inclusions, and have better compositional homogeneity. Virtual Frisch grid detectors were fabricated from crystals taken from a CdZnTeSe ingot that was grown by the traveling heater method. The detectors were fabricated from an as-grown ingot, bypassing the post-growth annealing process commonly practiced for industrial-grade CZT. The performances of the detectors were studied with different Frisch grid lengths using an amplifier shaping time ranging from 1–6 µs. The detectors showed high-quality spectroscopic performance with an as-measured energy resolution of ~1.1% at 662 keV for an optimum Frisch grid length of 3 mm. The charge collection was observed to enhance for longer Frisch grids.

47 OTHER INSTRUMENTATION↗

Multimodal characterization of Te inclusions in Cd 1−x Zn x Te and Cd 1−x Zn x Te 1−y Se y for gamma and X-ray detectors

While CdZnTe (CZT) and CdZnTeSe (CZTS) semiconductors have emerged as compounds for room-temperature gamma and X-ray detection materials, they continue to be constrained by the formation of Te-inclusion defects generated during the growth and post-growth phases of the material, which adversely affect the detector performance. We demonstrate the utility of multimodal microscopic imaging and analysis for the characterization of the optical and electronic properties of Te inclusions in CZT and CZTS crystals at both micron and nanometer length scales. Having first identified regions with micron-scale Te inclusions using confocal Raman microscopy techniques, optically coupled infrared scattering near-field optical microscopic mapping was performed to map the distribution of these inclusions with nanometer spatial resolution and correlate the presence of Te inclusions in the matrix with other properties. Kelvin probe force microscopy was then utilized to characterize the variations of the work function associated with the presence of Te inclusions. Here, we observe an increase of ~ 240 mV in the work function associated with Te inclusions compared to the bulk CZT/CZTS crystals. Additionally, we observe that individual bulk grains in CZT can exhibit slight potential variations. Our findings develop a portrait of the charge trapping mechanisms in CZT and CZTS that act to degrade detector performance, while the demonstration of these combined microscopy techniques provides a new analytical tool that can be utilized for further optimization of the detector performance for these semiconducting compounds.

36 MATERIALS SCIENCE↗

Local rare-earth dopant structure in a complex-oxide/semiconductor heterojunction: Molecular beam epitaxy grown Yb-doped SrTiO3 on Si(001)

We have investigated the structural and electronic properties of Yb-doped SrTiO3/Si(001) grown by molecular beam epitaxy. Other rare-earth donor dopants that result in n-type conductivity typically substitute for Sr at the A-sites in the perovskite lattice. In contrast, Yb has been found to substitute predominantly for Ti at the perovskite B-sites based on data from atomically resolved scanning transmission electron microscopy and spectroscopy, as well as extended x-ray absorption fine structure. Yb exhibits two distinct charge states as determined by x-ray absorption spectroscopy and associated modeling, +2.7 and +2.1. These aliovalent substitutional dopants are compensated by donor electrons from oxygen vacancies that form during epitaxial film growth. An atom beam flux mismatch was present during film depositions because it was assumed that Yb would occupy A-sites, leading to a flux matching formula given by Yb + Sr = Ti. However, the formation of YbTi rather than YbSr results in Sr vacancies and extraneous (i.e. non-lattice) Ti atoms in the films, or on the film surfaces. The presence of these defects, together with oxygen vacancies, leads to deep-level electron traps that were detected by resonant photoemission and much higher sheet resistance than that associated with, for instance, La-doped films.

Chambers, Scott A. (ORCID:000000025415043X)↗

Optical coherence tomography imaging of plant root growth in soil

Complex interactions between roots and soil provide the nutrients and physical support required for robust plant growth. Yet, visualizing the root-soil interface is challenged by soil’s opaque scattering characteristics. In this paper, we describe methods for using optical coherence tomography (OCT) to provide non-destructive 3D and cross-sectional root imaging not available with traditional bright field microscopy. OCT is regularly used for bioimaging, especially in ophthalmology where it can detect retinal abnormalities. Prior use of OCT in plant biology has focused on surface defects of above ground tissues, predominantly in food crops. Our results show OCT is also viable for detailed, in situ study of living plant roots.

59 BASIC BIOLOGICAL SCIENCES↗

Three-dimensional broadband nonlinear phased array imaging

System include an ultrasonic transducer configured to couple to a nondestructive testing (NDT) sample and configured to produce and direct an ultrasonic probe wave at a selected frequency into a subsurface region of the NDT sample, a 3D laser scanning vibrometer configured to direct a detection beam in a scan area on a surface of the NDT sample and to receive a return beam from the scan area, and to detect, based on the return beam, a 3D motion of the surface across a wideband frequency range, and a processor, and a memory configured with instructions that, when executed by the processor, cause the processor to produce sub-surface image data of the NDT sample at multiple harmonics of the selected frequency in the wideband frequency range based on the detected 3D surface motion, wherein the sub-surface image data describes a nonlinear defect response produced in the NDT sample by interaction of the ultrasonic probe wave with the subsurface region.

Remillieux, Marcel↗

Probing boron vacancy defects in hBN via single spin relaxometry

Spin defects in solids offer promising platforms for quantum sensing and memory due to their long coherence times and optical addressability. Here, we integrate a single nitrogen-vacancy (NV) center in diamond with scanning probe microscopy to detect, read out, and spatially map spin-based quantum sensors at the nanoscale. Using the boron vacancy ($V$$^{–}_{B}$) center in hexagonal boron nitride—an emerging two-dimensional spin system—as a model, we detect its electron spin resonance indirectly via changes in the spin relaxation time (T 1 ) of a nearby NV center, eliminating the need for optical excitation or fluorescence detection of the $V$$^{–}_{B}$. Cross-relaxation between NV and $V$$^{–}_{B}$ ensembles significantly reduces NV T1, enabling quantitative nanoscale mapping of defect densities beyond the optical diffraction limit and clear resolution of hyperfine splitting in isotopically enriched h 10 B 15 N. Our method demonstrates interactions between spin sensors in 3D and 2D materials, establishing NV centers as versatile probes for characterizing otherwise inaccessible spin defects.

Quantum metrology↗

Role of Selenium in CdZnTeSe as a Defect Engineering Agent

Cadmium zinc telluride (CdZnTe) with 10 atomic % Zn has been the material of choice for room-temperature semiconductor compact X- and gamma-ray detector applications for over three decades. Despite its commercial success as the most desirable room-temperature semiconductor radiation detection material, CdZnTe (CZT) suffers from a lack of compositional homogeneity on both the micro- and macroscales and the presence of high concentrations of performance-limiting defects such as subgrain boundary networks (dislocation walls) and secondary phases (Te-rich inclusions). Random distributions of these defects in the CZT matrix result in the spatial inhomogeneity of the material’s charge-transport properties. The recently discovered quaternary Cd x Zn 1-x Te 1-y Se y (CZTS) has experienced remarkable advances in its material properties, with highly reduced defects and higher compositional homogeneity. This book chapter focuses on the presence of performance-limiting defects in CZT that have thus far hindered the yield and cost of high-quality detectors and restricted their widespread deployment for a variety of potential applications, particularly for their use as large-volume gamma detectors, where the demands on material perfection are significantly greater. This chapter also provides an overview of the recent developments in the quaternary material CZTS, particularly the effects of selenium (Se) in the CZTS matrix on the defect engineering of the quaternary alloy material and the advancement of CZTS as a potential next-generation detector operable at room temperature.

Roy, Utpal N.↗

High Throughput In-Line Coating Metrology Development for Solid Oxide Fuel Cell Manufacturing

Coatings play key roles in solid oxide fuel cell (SOFC) stack durability. For example, diffusion barrier coatings on Cr-containing interconnect and balance of plant (BOP) components protect electrodes from Cr poisoning over the long operational lifetimes (>10,000 hours) of the fuel cell stack. Common defects in coatings, such as cracks, pinholes, and porosity, result in a failure to protect the electrodes, resulting in shorter operational lifetime and thus higher cost. It is very unlikely, even in the best coating process, that all these defects can be mitigated, hence identifying critical defects in parts, and removing defective parts from production before they can damage the stack, becomes paramount. Furthermore, these quality control techniques must be operational in the production/assembly line (in-line), i.e., high throughput and non-destructive, and cost effective. Redox Power Systems, LLC (Redox) together with the National Renewable Energy Laboratory (NREL) developed much needed high throughput, in-line metrology techniques for protective coatings. The overall goal of the project is to lower cost while increasing robustness, reliability, and endurance of SOFC stacks. To accomplish this, we had several objectives, including: to identify key coating and substrate defects that lead to coating failure through the use of detailed characterization methods (e.g., microscopy, XRD, EDS, electrochemistry); to assess capabilities of in-line metrology techniques, e.g., optical profilometry (Redox) and thermography (NREL), to probe these defects, or evidence thereof; demonstrate long-term performance of “defect-free” protective coatings, as identified by in-line metrology, in solid oxide fuel cell (SOFC) stack operation. In the first part of this project, the ability to identify key defects expected to lead to coating and SOFC degradation using in-line metrology tools were evaluated. Coated interconnect samples with controlled defect types and populations were tested under conditions similar to SOFC operation, followed by detailed post-test analysis to reveal the defects responsible for observed degradation. In the second part of the project, the optimal in-line metrology techniques and methodologies were used to map the defect distribution in full-size interconnects with critical defects intentionally allowed to exist in some cases. These interconnects underwent SOFC testing for extended periods (up to ~3,000 hours) followed by post-test analysis to evaluate the effectiveness of in-line metrology techniques in mitigating MCO coating related degradation. Key accomplishments in this project included the following: Demonstrated ASR of < 0.05 ohm-cm 2 at 650 °C for 1,000 hours with low defect (determined by in-line metrology) interconnect samples (average ASR=37 milliohms-cm 2 after over 1,000 hours). Demonstrated that low defect coatings on interconnects (as screened using in-line metrology) have low volatilization of chromium at ~650 °C for 1,000 hours as detected using Cr-getter material (< 5 at% increase above baseline); 1022 hour duration tests under humidified, elevated temperature (750 °C rather than 650 °C) compared a base case against different coating thicknesses. Demonstrated capability to identify initial key defects of interest with in-line metrology techniques using up to 8 cm by 10 cm having coatings with and without intentional defects of interest using thermal imaging and optical profilometry. Correlated key defects identified using metrology techniques with observed coating performance (e.g., ASR and Cr volatility). Conducted several 4 cm by 4 cm cell tests using MCO-interconnects that were pre-screened using some of the metrology techniques developed in the project (e.g., optical profilometry). An analysis of ASR measurements were able to show that defect-free coatings resulted in the anticipated performance in the cell tests.

01 COAL, LIGNITE, AND PEAT↗

Identify and Assess Technical Challenges in Safeguards Measurements of Spent Advanced Reactor Fuels

Advanced reactor (AR) designs use various nuclear fuel types that can be significantly different than conventional light-water reactor (LWR) fuels, including differences in sizes, compositions, and chemical forms (e.g., oxide, carbide, metal). Nearly all the proposed AR fuels use high-assay low-enriched uranium (HALEU), which will have higher enrichments (5–20 wt% 235 U) than LWR fuels (currently limited to <5 wt% 235 U). In advance of the wide use of these new fuel types around the world, international safeguards organizations such as the International Atomic Energy Agency (IAEA]) are working with some of the AR vendors to formulate safeguards approaches for these AR fuel cycles. As part of the overall safeguards approach, it is important to identify the potential technical challenges in performing safeguards verification measurements of these AR fuels (both fresh and spent fuels) in advance of the widespread adoption of these new fuel types, because new safeguards technologies can take several years to develop, test, and approve for use. This report documents work performed in fiscal year 2024 based on modeling and simulation to assess the performance of the existing safeguards measurement technologies for irradiated or spent AR fuel elements or items. This work is a continuation of the work performed in fiscal year 2023 that focused on fresh AR fuels. Spent AR fuels have a distinct difference from their LWR counterparts: unlike the spent LWR fuels typically stored in a water-filled pool, some spent AR fuels—such as tristructural-isotropic (TRISO)-based fuels—will most likely be stored in air-filled hot cells. Because most safeguards measurements on spent fuel performed to date have been conducted under water, the air-filled hot cell environment could present unique challenges to safeguards measurements. Fork detector (FDET) and Cerenkov viewing device (CVD) systems have been the two primary instruments used by the IAEA for several decades to measure spent LWR fuel assemblies stored in pools for safeguards verification purposes. Because the lower refractive index of air causes Cerenkov light to be of lower intensity in air than in water, existing CVDs are likely unable to perform safeguards verification measurements for spent fuel stored in an air-filled hot cell, as is the case for the TRISO-based spent fuel elements (e.g., pebbles, graphite fuel blocks). Unlike FDET measurements, CVD measurements do not require fuel be moved, so they are a simpler and faster to take than FDET measurements. The inability to perform CVD measurements on the TRISO-based AR fuel types presents a major technical challenge in the effort to use existing technology to perform safeguards measurements on spent AR fuels. This study was mainly conducted through the modeling and simulation of an FDET or an FDET-like system on five spent AR fuel types, including one metallic fuel type and four TRISO-based fuel types in both pebble and graphite block forms in their respective storage configurations and environments. Because the various AR fuel types have significantly different dimensions, FDET systems must be adapted to accommodate them. Partial defect tests were also simulated in this study to assess the FDET’s ability to detect potential fuel diversions. The FDET measures the fuel’s total passive neutron and gamma emissions. The simulated FDET results from spent AR fuel items are compared against results from a typical spent pressurized water reactor (PWR) assembly. High-purity germanium (HPGe) gamma detector measurements were also simulated for the spent AR fuel types and the PWR assembly because the signature photopeaks have been used in LWR safeguards verifications, although HPGe is usually not used to detect diversions because of the fuel’s self-attenuation effects on those photopeaks. The results indicate that these detectors have significant challenges in performing safeguards measurements of the spent AR fuel items, including incompatibilities between AR fuel items and existing FDETs, lower neutron count rates, lower sensitivities to fuel diversions in certain AR fuel items, and significantly higher interference from a neighboring fuel item when the measurement is performed in air. These results suggest that an alternative technology or significant and timely technology development is needed to perform adequate safeguards measurements of some of these AR fuel items.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Automated Defect Identification for Tri-structural Isotropic Fuels (AUDIT)

During the manufacture of tri-structural isotropic (TRISO)-coated nuclear fuel particles, the potential exists for the formation of internal fissure defects in the uranium oxycarbide (UCO) kernels. These fissures result in a defective fuel particle that can fracture during subsequent fuel processing. Therefore, it is necessary to detect the presence of fissured kernels in a batch to determine if the batch meets specification prior to blending with other batches and upgrading processes. Previous attempts at identifying fissures involved manual inspection of micrographs of UCO fuel kernel cross-sections. This process is tedious, time-consuming and may introduce counting errors making it a good candidate for automation. This work presents a method for the automated detection of fissures in UCO kernels. Image segmentation is used for the extraction of relevant features in the micrographs which then serve as the input to a convolutional neural network used to automatically distinguish between fissured and non-fissured kernels.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Melting and defect transitions in FeO up to pressures of Earth’s core-mantle boundary

The high-pressure melting curve of FeO controls key aspects of Earth’s deep interior and the evolution of rocky planets more broadly. However, existing melting studies on wüstite were conducted across a limited pressure range and exhibit substantial disagreement. Here we use an in-situ dual-technique approach that combines a suite of >1000 x-ray diffraction and synchrotron Mössbauer measurements to report the melting curve for Fe 1-x O wüstite to pressures of Earth’s lowermost mantle. We further observe features in the data suggesting an order-disorder transition in the iron defect structure several hundred kelvin below melting. This solid-solid transition, suggested by decades of ambient pressure research, is detected across the full pressure range of the study (30 to 140 GPa). At 136 GPa, our results constrain a relatively high melting temperature of 4140 ± 110 K, which falls above recent temperature estimates for Earth’s present-day core-mantle boundary and supports the viability of solid FeO-rich structures at the roots of mantle plumes. The coincidence of the defect order-disorder transition with pressure-temperature conditions of Earth’s mantle base raises broad questions about its possible influence on key physical properties of the region, including rheology and conductivity.

58 GEOSCIENCES↗