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At least 703 records · Page 39

Electronic Excitation‐Driven β‐Ga 2 O 3 Metastability Transformation and Self‐Organization Mechanism: β→κ/γ/δ Phases

Here, irradiation-driven multiphase self-organization presents emergent opportunities for the customization of nanoscale engineering properties, dynamically tuning strain-field distributions and interfacial electronic structures. Responding to intense electronic excitation-induced energy deposition, the dominant phase transformations, with varying Gibbs free energy $Δ,G^o_f$ are confirmed as β → κ → γ → δ that are located in specific microregions for Gallium (III) oxide (Ga 2 O 3 ), as follows: (i) Surface-localized interstitial accumulation under compressive stress triggers β → δ via semi-coherent interface formation. (ii) Tensile stress within latent tracks drives vacancy-mediated oxygen layer truncation (4/12 periodicity along ⟨0001⟩), stabilizing coherent 4H (ABCB) κ and 3C (ABC) β (ABC) interfaces through strain-compensated octahedral distortion. (iii) Screw dislocation-mediated lattice relaxation induces β → γ via cation disordering (Ga 3+ occupancy at β-interstitial sites), forming metastable spinel γ with mixed occupancy across 16d/8a Wyckoff sites. Irradiation-driven β-Ga 2 O 3 →κ/γ/δ transitions, as mechanistically revealed via inelastic thermal spike (i-TS) calculations and molecular dynamics simulations, induce defect-mediated nonlinear photoresponse, critical for optoelectronic engineering.

Han, Xinqing [Shandong Univ., Jinan (China)]↗

Localized keyhole pore prediction during laser powder bed fusion via multimodal process monitoring and X-ray radiography

Systematic fault detection and control during laser powder bed fusion (L-PBF) has been a long-standing objective for system manufacturers and researchers in the additive manufacturing (AM) industry. This manuscript investigates a data fusion approach for detection of keyhole porosity formation during laser irradiation of Ti-6Al-4V substrates by concurrent recording of thermally induced optical emission measured using both off-axis and coaxial photodiode sensors, and acoustic emission. Subsurface defect formation was monitored via high-speed synchrotron X-ray imaging at 20,000 frames per second, enabling temporal registration of keyhole pore formation events to the monitoring signals at a resolution of 50 µs. We developed data fusion machine learning (ML) models for localized prediction of keyhole pore formation at various time scales ranging from 0.5 ms to 2 ms. The signal segments were featurized using two independent approaches: (1) power spectral density (PSD) and (2) highly comparative time series analysis (HCTSA) framework. The extracted features from different sensor modalities were fused together to construct a multimodal feature space and sequential feature selection was used to determine the most informative features for training the ML models. The predictive performance was evaluated for three classifying algorithms: Support Vector Machine (SVM), K-Nearest Neighbor (KNN), and Gaussian Naive Bayes (GNB). As a result, pore formation events were predicted with up to 0.95 F1-score, 1.0 recall and 0.94 accuracy. The most heavily weighted features indicate that model performance is chiefly governed by the acoustic monitoring signal, with a secondary contribution from the optical emission sensors.

36 MATERIALS SCIENCE↗

Three-dimensional strain imaging of irradiated chromium using multi-reflection Bragg coherent diffraction

Abstract Radiation-induced materials degradation is a key concern in limiting the performance of nuclear materials. The formation of nanoscale void and gas bubble superlattices in metals and alloys under radiation environments can effectively mitigate radiation-induced damage, such as swelling and aid the development of next generation radiation tolerant materials. To effectively manage radiation-induced damage via superlattice formation, it is critical to understand the microstructural changes and strain induced by such superlattices. We utilize multi-reflection Bragg coherent diffraction imaging to quantify the full strain tensor induced by void superlattices in iron irradiated chromium substrate. Our approach provides a quantitative estimation of radiation-induced three-dimensional (3D) strain generated at the microscopic level and predicts the number density of defects with a high degree of sensitivity. Such quantitative evaluation of 3D strain in nuclear materials can have a major impact on predicting materials behavior in radiation environments and can revolutionize design of radiation tolerant materials.

36 MATERIALS SCIENCE↗

Lithium - An impurity of interest in radiation effects of silicon.

Study of the introduction and annealing of defects produced in lithium-diffused float-zone n-type silicon by 30-MeV electrons and fission neutrons. The introduction rate of recombination centers produced by electron irradiation is dependent on lithium concentration and for neutron irradiation is independent of lithium concentration. The introduction rate of Si-B1 centers also depends on the lithium concentration. The annealing of electron- and neutron-produced recombination centers, Si-B1 centers, and Si-G7 centers in lithium-diffused silicon occurs at much lower temperatures than in nondiffused material.

Naber, J. A.↗

Impact of amorphous pockets on displacement damage evolution in silicon

Silicon has long been known to exhibit amorphization in response to heavy particle bombardment. For doses below the total amorphization threshold, partial amorphization is observed in the form of scattered amorphous pockets. While extensive research has gone into modeling the formation and evolution of amorphous pockets in response to irradiation, no studies yet investigate their impact on the evolution of other damage such as interstitial supersaturation and clustering. In this study, we survey the impact of amorphous pockets on defect evolution in silicon when treated as static sinks. MD is first used to show that amorphous pockets provide energetically favorable sites for point defects relative to the crystalline bulk, supporting the hypothesis that they act as sinks. A 0-D cluster dynamics model is then constructed, taking an interstitial clustering model from the literature and including amorphous pockets as a sink species. We conduct our survey for temperatures between 30 and 400 °C and sink strengths between 1 to 6 x 10 10 cm −2 . Both implantation- and radiation-induced damage states are investigated using interstitial and vacancy concentrations as initial condition variables. We find that, due to the differing migration rates of the interstitial and the vacancy, amorphous pockets have a non-monotonic impact on the final damage state depending on the effective sink strength of the amorphous pockets, resulting in increased damage formation in regimes of intermediate amorphization. In conclusion, this result emphasizes the important role of amorphous pockets in governing the evolution of damage in partially amorphized crystalline materials.

36 MATERIALS SCIENCE↗

High-Entropy Alloys for Accelerator Beam Window Applications

Development of novel high-entropy alloys (HEAs) is currently underway for potential use as beam windows in future multi-megawatt target systems at Fermilab. HEAs encompass a new class of materials with a vast design space allowing for material properties to be tailored for particular applications and to potentially offer improved resistance to beam-induced radiation damage and thermal shock effects. The alloy systems being studied consist of several compositions of AlCoCrMnTiV with 4 6 component elements. These alloys are all predicted by CALPHAD simulation to have a single-phase BCC crystal structure and low density, with some compositions displaying ordered, nanoscale precipitates. This presentation will briefly discuss alloy design and synthesis before giving a detailed description of the characterization studies of these HEAs in both the pristine state and post-irradiation by low-energy heavy ions to high damage levels. Electron microscopy techniques to quantify elemental homogeneity and composition, determine grain size, shape, and orientation, and quantify lattice parameters, defect structures and precipitate phases are all being used to study alloy microstructures. Mechanical properties of the alloys at the microscale will be reported. The evolution of these properties as a function of radiation damage will also be described. Bulk thermal characteristics of these HEAs have been tested to measure specific heat capacity and coefficient of thermal expansion as a function of temperature. To determine bulk tensile properties a miniature tensile testing apparatus is under development; it s commissioning will be covered briefly. The talk will conclude with our plans for alloy down-selection.

Burleigh, A. [Fermilab]↗

Distinctive features of fluorescence and waveguides in magnesium aluminate spinel crystals driven by structural discrepancy

Transparent polycrystalline ceramics are of significant importance for a wide range of scientific and industrial applications. Developing a deeper understanding of their thermodynamic behavior is essential for achieving their maximum output performance in technological applications. This study provides a systematic investigation into the thermal excitation-induced fluorescence kinetics and waveguide characteristics of Magnesium Aluminate Spinel (MgAl 2 O 4 ) single crystals, with a focus on the intricate relationship between structure and properties. High-temperature extreme environments through irradiation with swift heavy ions 645.0 MeV Xe and 352.8 MeV Fe ions were created; the atomic deposition energy threshold (E th ) associated with disorder morphologies was assessed between 0.91 and 0.99 eV atom –1 . The track prediction model was developed to support the theoretical prediction of track formation. Electronic energy loss (E ele ) disrupts the balance of the initial structure through the thermal spike effect, leading to the formation of absorption-related F and F + color centers. These defects enhance photoluminescence in the visible spectrum and result in an effective modulation of the intrinsic bandgap. Moreover, as ion beams penetrate into the material, the uneven damage distribution induces the formation of waveguide structures. In conclusion, these findings provide valuable insights into the fabrication of functional devices through irradiation technologies and the structural changes of MgAl 2 O 4 at high temperatures within extreme environments.

36 MATERIALS SCIENCE↗

Computationally guided experimental validation of divacancy defect formation in 4H-SiC

Recent research into solid-state qubits for quantum information science has focused on optically addressable spin defects such as the negatively charged nitrogen-vacancy center in diamond and the neutrally charged divacancy (VV) in 4H-SiC as scalable quantum sensors and networking qubits. Within this context, direct investigations of the structural origin and defect formation dynamics of a sub-set of the VV center in 4H-SiC remain lacking. Here, we take a systematic experimental approach guided by predictions from first-principles simulations to gain a thorough mechanistic understanding of the VV defect formation and control in 4H-SiC. We study the effect of annealing time and temperature on VV formation in high-purity semi-insulating 4H-SiC samples following electron irradiation. Three different temperatures (1123, 1273, and 1473 K) and annealing duration (from 0.5 to 72 h) are chosen to explore VV formation in different regions. We find that samples annealed at 1273 K give the highest VV-related photoluminescence (PL) intensities, in agreement with the prediction from first-principles calculations. Furthermore, the logarithmic dependence of VV-related PL intensities on the annealing duration at 1273 K indicates that 1273 K provides sufficient thermal energy for silicon vacancy migration but not for VV migration. Together, these results suggest that efficient VV formation occurs above the V Si migration temperature and below the VV migration threshold.

74 ATOMIC AND MOLECULAR PHYSICS↗

Photonic and Opto-Electronic Applications of Polydiacetylene Films Photodeposited from Solution and Polydiacetylene Copolymer Networks

Polydiacetylenes (PDAS) are attractive materials for both electronic and photonic applications because of their highly conjugated electronic structures. They have been investigated for applications as both one-dimensional (linear chain) conductors and nonlinear optical (NLO) materials. One of the chief limitations to the use of PDAs has been the inability to readily process them into useful forms such as films and fibers. In our laboratory we have developed a novel process for obtaining amorphous films of a PDA derived from 2-methyl4-nitroaniline using photodeposition with Ultraviolet (UV) light from monomer solutions onto transparent substrates. Photodeposition from solution provides a simple technique for obtaining PDA films in any desired pattern with good optical quality. This technique has been used to produce PDA films that show potential for optical applications such as holographic memory storage and optical limiting, as well as third-order NLO applications such as all-optical refractive index modulation, phase modulation and switching. Additionally, copolymerization of diacetylenes with other monomers such as methacrylates provides a means to obtain materials with good processibility. Such copolymers can be spin cast to form films, or drawn by either melt or solution extrusion into fibers. These films or fibers can then be irradiated with UV to photopolymerize the diacetylene units to form a highly stable cross-linked PDA-copolymer network. If such films are electrically poled while being irradiated, they can achieve the asymmetry necessary for second-order NLO applications such as electro-optic switching. On Earth, formation of PDAs by the above mentioned techniques suffers from defects and inhomogeneities caused by convective flows that can arise during processing. By studying the formation of these materials in the reduced-convection, diffusion-controlled environment of space we hope to better understand the factors that affect their processing, and thereby, their nature and properties. Ultimately it may even be feasible to conduct space processing of PDAs for technological applications.

Paley, Mark S.↗

Investigation of the irradiation effects in additively manufactured 316L steel resulting in decreased irradiation assisted stress corrosion cracking susceptibility

While additive manufacturing (AM) is an area of increasing interest to the nuclear industry, there are significant research and development needs prior to successful implementation of additively manufactured components into reactors. AM steel behaves differently than traditional wrought material, as has been observed in numerous mechanical testing studies. The nuclear industry must also understand the material response to irradiation. This work examines the irradiation damage and the irradiation assisted stress corrosion cracking behavior (IASCC) of both proton irradiated AM and wrought 316L steel. For IASCC testing, specimens were strained to 4% plastic strain in a simulated boiling water reactor environment (288°C, 0.2 µS/cm). Transmission and scanning electron microscopy, confocal microscopy, and X-ray computed tomography were used to examine coupons of the material as well as tensile bars used in the IASCC testing. This work found that the wrought 316L was more susceptible to IASCC than the AM steel, however, some IASCC was observed in the AM steel when tested with the tensile axis parallel to the build direction. Electron microscopy has shown significantly fewer radiation induced voids formed in the AM steel. While the pre-existing pore network in the AM steel may act as a sink to point defects, this is not expected to be the major factor in the reduced swelling observed in the AM steel. The lower density of radiation induced voids was expected to contribute to the IASCC resistance by decreasing the localization of deformation in the irradiated specimens, however, severity of localized deformation in AM steel, measured in dislocation channel spacing and height, was similar or more severe to that found in wrought. In conclusion, the presence of severe cracking in the wrought specimens did not allow for a direct comparison of localized deformation severities between the AM and wrought steel.

Additive manufacturing↗

Raman signatures from age-dating PuO 2 since last calcination

The self-irradiation of PuO 2 has been shown to affect the attributes of fifteen vibrational bands in the Raman spectrum. The vibrational bands correspond to the Raman allowed vibrational mode T 2g , overtones, defects, and bands from electronic origin. Defects in the crystal lattice from low-calcination temperature and alpha decay origins are responsible for the changes in the band attributes (band position, full-width half maximum (FWHM), intensity). Crystal lattice defects are also responsible for the growth of the defect bands. The temporal behavior of the vibrational bands can be used to estimate the age of the material since last calcination. Laser annealing was used to reset the material to full crystallinity prior to the aging study. 240 PuO 2 , with an alpha decay rate of 3.67 greater than the decay rate of 239 PuO 2 , was primarily used to assess the alpha decay-induced damage within 3 years. The aging study focused on the time-dependent properties of the T 2g band and the growth of defect bands. The FWHM of the T 2g band and the ratio of the areas of the defect bands/T 2g band were measured through a time period in excess of 3 years. The data from this study were found very close to the data describing the temporal evolution of the lattice constant measured with the X-ray diffraction (XRD) technique. The local physical properties of the material measured with Raman spectroscopy and the lattice parameter constant measured with XRD indicates a strong correlation between the two techniques. Although both techniques provide similar age-dating information, in contrast to the few milligram quantities required for XRD, Raman spectroscopy requires a 10 µm diameter PuO 2 particle to provide an estimate of the material age since last calcination.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fundamental Phenomena and Applications of Swift Heavy Ion Irradiations

This review concentrates on the specific properties and characteristics of damage structures generated with high-energy ions in the electronic energy loss regime. Irradiation experiments with so-called swift heavy ions (SHIs) find applications in many different fields, with examples presented in ion-track nanotechnology, radiation hardness analysis of functional materials, and laboratory tests of cosmic radiation. The basics of the SHI-solid interaction are described with special attention to processes in the electronic subsystem. The broad spectrum of damage phenomena is exemplified for various materials and material classes, along with a description of typical characterization techniques. This review also presents state-of-the-art modeling efforts that try to account for the complexity of the coupled processes of the electronic and atomic subsystems. Lastly, a brief discussion at the end of this review on SHI phenomena induced by fission fragments in nuclear materials will highlight the relevance of energetic ion irradiation in nuclear technology applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Cluster dynamics simulation of xenon diffusion during irradiation in UO 2

Diffusion of fission gas in UO 2 nuclear fuel impacts several important performance metrics, such as fission gas release, swelling, and thermal conductivity. Current empirical models of fission gas release have significant uncertainty, some of which derives from the bulk diffusion rate and its dependence on, for example, fuel chemistry and irradiation. In this work, we have applied the previously-developed Free Energy Cluster Dynamics (FECD) methodology in the code Centipede to calculate xenon cluster concentrations in UO 2 under intrinsic (high temperature) and irradiation-enhanced (intermediate temperature) conditions in order to develop a model of the xenon diffusion coefficient based on the atomic scale mechanisms responsible for transport. While the diffusion mechanism for xenon in UO 2 is adequately described by the Xe + U 2 O vacancy cluster for intrinsic conditions, a similar process is not capable of capturing measured in-pile fission gas diffusivity at intermediate temperatures. Therefore, a different diffusion mechanism must dominate under this regime. Using calculated atomistic data, we have shown that irradiation-enhanced diffusion at intermediate temperatures occurs via the larger Xe + U 4 O y vacancy clusters, which have lower migration barriers and increase in concentration by several orders of magnitude compared to intrinsic conditions. This mechanism is enabled by the increased uranium vacancy concentration under irradiation due to Frenkel pair production. In addition, the fast migration of uranium interstitials with two attached oxygen interstitials lowers the total uranium interstitial concentration through reactions with sinks. This allows the extended defects, such as Xe + U 4 O y vacancy clusters, to maintain high concentrations by limiting annihilation with attached vacancies. Furthermore, predictions using the Xe + U 4 O y diffusion mechanism are in good agreement with experiment, albeit with some differences in the Arrhenius slope, which we believe may be related to either experimental or model parameter uncertainty. Lastly, an analytical expression suitable for application in fuel performance simulations was derived to capture the predictions of the Centipede simulations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Inducing a tunable skyrmion-antiskyrmion system through ion beam modification of FeGe films

Abstract Skyrmions and antiskyrmions are nanoscale swirling textures of magnetic moments formed by chiral interactions between atomic spins in magnetic noncentrosymmetric materials and multilayer films with broken inversion symmetry. These quasiparticles are of interest for use as information carriers in next-generation, low-energy spintronic applications. To develop skyrmion-based memory and logic, we must understand skyrmion-defect interactions with two main goals—determining how skyrmions navigate intrinsic material defects and determining how to engineer disorder for optimal device operation. Here, we introduce a tunable means of creating a skyrmion-antiskyrmion system by engineering the disorder landscape in FeGe using ion irradiation. Specifically, we irradiate epitaxial B20-phase FeGe films with 2.8 MeV Au 4+ ions at varying fluences, inducing amorphous regions within the crystalline matrix. Using low-temperature electrical transport and magnetization measurements, we observe a strong topological Hall effect with a double-peak feature that serves as a signature of skyrmions and antiskyrmions. These results are a step towards the development of information storage devices that use skyrmions and antiskyrmions as storage bits, and our system may serve as a testbed for theoretically predicted phenomena in skyrmion-antiskyrmion crystals.

74 ATOMIC AND MOLECULAR PHYSICS↗

Radiation effects in Ga(0.47)In(0.53)As solar cells

The effects of irradiating Ga(0.47)In(0.53)As p-i-n junctions with 1 MeV electrons were measured using Deep Level Transient Spectroscopy (DLTS) and both dark and illuminated (1 sun, air mass zero (AM0)) current-voltage (I-V) measurements. The I-V measurements were made over the range 100K less than T less than 350K. Temperature coefficients of the Ga(0.47)In(0.53)As photovoltaic parameters are presented which follow the same general behavior as other solar cell materials (e.g. Si and GaAs). Fits of the dark I-V data to the two term diode equation before irradiation were satisfactory, yielding an estimated band-gap energy of 0.79 eV. The recombination component of the dark current was found to increase linearly with fluence. DLTS detected two radiation-induced defect levels one shallow (E(sub c)-0.10 eV) and one near mid-gap (E(sub c)-0.29 eV), and it is the near mid-gap level which is expected to be the cause of the dark current increase. The radiation-induced degradation of the open circuit voltage is shown to be accurately predicted from the dark I-V measurements. The degradation of the open circuit voltage dominated the radiation response of the photovoltaic parameters while the short circuit current was only moderately degraded. This behavior is qualitatively explained in terms of the base thickness and dopant level. Appropriate changes in the device structure are suggested which should increase the radiation resistance. Isochronal thermal annealing induced recovery in the photovoltaic parameters at approximately 400K, coinciding with an annealing stage of the near mid-gap defect level.

Walters, R. J.↗

Efficient high-fidelity TRISO statistical failure analysis using Bison: Applications to AGR-2 irradiation testing

The ability of tri-structural isotropic (TRISO) fuel to contain fission products is largely dictated by the quality of the manufacturing process, since most of the fission product release is expected to occur due to coating layer failure in a small number of particles containing defects. The Bison fuel performance code has capabilities to predict failure in individual particles, accounting for the presence of defects, and to apply statistical analysis methods to compute the probability of failure in a set of fuel particles. Bison has recently undergone significant development both to improve its physical representations of fuel particle behavior and to improve the efficiency of its statistical failure calculations. Physical model improvements include new capabilities to account for the pressure generated by fission gases on inner pyrolytic carbon (IPyC) crack surfaces and to use local material coordinate orientation to accurately incorporate the anisotropy in the material properties in aspherical particles. To improve statistical modeling efficiency, a direct integration approach which involves directly integrating the failure probability function associated with statistically varying parameters has been developed. The direct integration approach is much more efficient than the Monte Carlo (MC) schemes commonly employed, and allows Bison to directly run high-dimensional fuel performance models, which improves the accuracy of failure probability calculations. Finally, a set of benchmark problems is considered here to compare the MC and direct integration approaches, and a statistical failure analysis of compacts in the Advanced Gas Reactor (AGR)-2 experiments is performed using the direct integration approach.

36 MATERIALS SCIENCE↗

Why are Buckyonions Round?

Multi-layered round carbon particles (onions) containing tens to hundreds of thousands of atoms form during electron irradiation of graphite. However. theoretical models or large icosahedral fullerenes predict highly faceted shapes for molecules with more than a few hundred atoms. This discrepancy in shape may be explained by the presence of defects during the formation of carbon onions. Here, we use the semi-empirical tight-binding method for carbon to simulate the incorporation of pentagon-heptagon defects on to the surface of large icosahedral fullerenes. We show a simple mechanism that results in energetically competitive derivative structures and a global change in molecular shape from faceted to round. Our results provide a plausible explanation of the apparent discrepancy between experimental observations or round buckyonions and theoretical predictions of faceted icosahedral fullerenes.

Bates, Kevin R.↗

In situ irradiation of spent nuclear fuels

To improve the economics of commercial nuclear reactors, nuclear vendors and utilities are seeking approval for increased burnup usage of the existing nuclear fleet. This is especially critical for meeting the clean energy initiative by the United States Government, Department of Energy (DOE). However, one of the key challenges the nuclear industry faces in this regard is that the regions exposed to high burnup and low temperatures exhibit a fine-grained microstructure with large bubbles known as high-burnup structure (HBS) [1]. The formation of HBS has been correlated to the diminished performance of the reactor, as well as fuel fragmentation and pulverization during transient and accidental conditions [2]. Therefore, it is paramount to understand the mechanisms for HBS formation along with its impact on the properties and performance of nuclear fuels. While existing programs, such as Nuclear Energy Advanced Modeling and Simulation (NEAMS) and Advanced Fuel Campaign (AFC) are focusing on evaluating the performance impact of HBS, the physical mechanisms contributing to HBS formation are still not fully understood. In addition, having predictive capabilities and sound understanding of the microstructural evolution of nuclear fuel is essential for accelerated development, qualification, and deployment of new nuclear materials and novel reactor designs for advanced nuclear reactors. There is a lack of consensus among researchers regarding the mechanisms leading to such restructuring observed in HBS. Grain subdivision due to polygonization versus recrystallization, continuous versus discrete recrystallization occurring in tandem or conjunction, etc., have been proposed and debated. In general, it is hypothesized that defect accumulation and dislocation interaction within the grains cause the realignment of dislocations into grain boundaries, leading to the new subgrain formation, which over time transforms into new grains. However, due to the lack of transient data, the importance of fission rate, irradiation, thermal, and stress history of the fuel on the restructuring could not be assessed. In situ microstructural evolution under various irradiation conditions is desired to bridge this gap. Alternatively, phase-field-based models have been developed to capture HBS formation via discrete recrystallization utilizing the classical nucleation approach [3–5]. However, in these models, the grain nucleation criteria are often defined based on empirical relations for burnup and fission gas density leading to dislocation density change. A mechanistic approach to capture the dislocation interaction with the microstructural features leading to grain subdivision is lacking.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗