arXiv subjects

Blas P. Uberuaga

Publications and source records attributed to Blas P. Uberuaga.

14 recordsLinked to original sources

arXiv2026

Achieving 5-angstrom-resolution diffraction contrast with an uncorrected electron probe and nanosized defect characterizations

Atomic-resolution micrographs remain limited in application due to small field of view and low numbers of recorded defects. Defect imaging with reliable statistics in transmission electron microscopy (TEM) relies heavily on diffraction contrast. However, with 200-300 kV electrons, low-curvature Ewald sphere limits diffraction resolution at ~5 nm. Here, we imaged defects with a forbidden condition in TEM and improved the resolution in diffraction contrast from 5 to 0.5 nm. The superiority of our equal-s method is demonstrated by the discovery of a novel phase and dislocation loop structure in steels, which have not been previously reported experimentally or theoretically. Our equal-s can largely replace the classical two-beam condition for defect study.

cond-mat.mtrl-sci↗

arXiv2026

Statistical Mechanics of Thermal Diffusion in Rough Energy Landscapes

Starting from a variational principle for mass transport, we present a broadly applicable statistical framework describing thermal diffusion in complex solids. We show that microscopic thermodynamic and kinetic fluctuations govern non-Arrhenius diffusion, with kinetic terms described by machine-learnable relative diffusion contributions. For vacancy diffusion in solid solutions, deviation from Arrheniusness may occur when ordering effects start to become important but at higher temperatures, approximately Arrhenius behavior can occur, aided by configurational entropy and competing energy fluctuations.

cond-mat.stat-mech↗

arXiv2026

Irradiation-induced amplification of electric fields at oxide interfaces as revealed by correlative DPC-STEM and DFT

Heterointerfaces are ubiquitous in modern devices, found in technologies ranging from microelectronics to structural components for energy applications. Many of these emerging technologies are found in applications such as satellites, batteries, and next generation nuclear reactors, that are subject to harsh environments. In some scenarios, multiple extreme conditions, such as irradiation and corrosion, act on the material simultaneously. Extending the lifetime of these technologies is dependent on a detailed understanding of how their component materials platforms and interfaces respond in extreme environments, where irradiation and corrosion may couple in unique ways, distinct from corrosion under ambient conditions. Oxides, which form readily over metal underlayers, can act as protective coatings; enhancing the robustness of oxide overlayers to protect underlying metal alloys is a potential avenue towards corrosion mitigation. Here we study the impact of irradiation-induced non-equilibrium defects on charge segregation and electric fields at and near multi-phase oxide heterointerfaces. We perform a detailed study of irradiated Fe2O3-Cr2O3 thin film heterostructures using first-principles DFT electronic structure modeling paired with 4D-STEM DPC and EELS techniques to measure nanoscale changes in electric fields. Our results show clear evidence that irradiation drives substantial modulation of interfacial electric fields that can be tailored by controlling the atomistic chemical structure of the oxide interface. We show that irradiation can selectively induce built-in electric fields, thereby altering their direction; this suggests a pathway to engineering protective oxide heterostructure overlayers that can electrically control the spatial distribution of defects, with significant implications for the design of corrosion-resistant materials for extreme environments.

cond-mat.mtrl-sci↗

arXiv2025

Critical Disconnect Between Structural and Electronic Recovery in Amorphous GaAs during Recrystallization

Understanding the evolution of structure and functionality through amorphous to crystalline phase transitions is critical for predicting and designing devices for application in extreme conditions. Here, we consider both aspects of recrystallization of irradiated GaAs. We find that structural evolution occurs in two stages, a low temperature regime characterized by slow, epitaxial front propagation and a high-temperature regime above dominated by rapid growth and formation of dense nanotwin networks. We link aspects of this structural evolution to local ordering, or paracrystallinity, within the amorphous phase. Critically, the electronic recovery of the materials is not commensurate with this structural evolution. The electronic properties of the recrystallized material deviate further from the pristine material than do those of the amorphous phase, highlighting the incongruence between structural and electronic recovery and the contrasting impact of loss of long range order versus localized defects on the functionality of semiconducting materials.

cond-mat.mtrl-sci↗

arXiv2025

Grain Boundary Anisotropy and Its Influence on Helium Bubble Nucleation, Growth, and Decohesion in Polycrystalline Iron

The accumulation of helium bubbles at grain boundaries (GBs) critically degrades the mechanical integrity of structural materials in nuclear reactors. While GBs act as sinks for radiation-induced defects, their inherent structural anisotropy leads to complex helium bubble evolution behaviors that remain poorly understood. This work integrates accelerated molecular dynamics simulations and a novel atomic-scale metric, the flexibility volume (V_f), to establish the interplay between GB character, helium segregation, and bubble growth mechanisms in body-centered cubic iron. We demonstrate that V_f, which incorporates both local atomic volume and vibrational properties, qualitatively predicts deformation propensity. Our results reveal that the atomic-scale segregation energy landscape dictates initial helium clustering and subsequent bubble morphology, with low-energy channels in tilt Σ5 boundary facilitating one-dimensional migration while isolated deep traps in twist Σ13 boundary promote larger, rounder bubble morphology. Critically, besides gradual bubble growth via trap mutation mechanism, we identify two distinct stress-relief mechanisms: loop punching in anisotropic tilt Σ5 boundary and interfacial decohesion in twist Σ11 boundary, with the dominant pathway determined by the interplay between bubble morphology and local mechanical softness. This study establishes a fundamental connection between GB crystallographic and energetical anisotropy and helium bubble evolution, providing critical insights for designing radiation-tolerant microstructures.

cond-mat.mtrl-sci↗

arXiv2024

Grain boundary metastability controls irradiation resistance in nanocrystalline metals

Grain boundaries (GBs) in polycrystalline materials are powerful sinks for irradiation defects. While standard theories assume that the sink efficiency of a grain boundary is defined solely by its character before irradiation, recent evidence conclusively shows that the irradiation sink efficiency is a highly dynamic property controlled by the intrinsic metastability of GBs under far-from-equilibrium irradiation conditions. In this paper, we reveal that the denuded (i.e., defect-free) zone, typically the signature of a strong sink, can collapse as irradiation damage accumulates. We propose a radiation damage evolution model that captures this behavior based on the emergence of a series of irradiation defect-enabled metastable GB microstate changes that dynamically alter the ability of the GB to absorb further damage. We show that these microstate changes control further defect absorption and give rise to the formation of a defect network that manifests itself as a net Nye-tensor signal detectable via lattice curvature experiments.

cond-mat.mtrl-sci↗

arXiv2024

Primary Defect Production in Doped Iron Grain Boundaries during Low Energy Collision Cascades

This study explores the intricate interactions between grain boundaries (GBs) and irradiation-induced defects in nanocrystalline iron, highlighting the role of dopants like copper. Utilizing molecular dynamics simulations, the research delineates how GB properties, such as GB energy and defect formation energies, influence the formation and evolution of defects in low energy collision cascades. It reveals that GBs not only augment defect production but also show a marked preference for interstitials over vacancies, a behavior significantly modulated by the cascade's proximity to the GB. The presence of dopants is shown to alter GB properties, affecting both the rate and type of defect production, thereby underscoring the complex interplay between GB characteristics, dopant elements, and defect dynamics. Moreover, the investigation uncovers that the structural characteristics of GBs play a crucial role in cascade evolution and defect generation, with certain GB configurations undergoing reconfiguration in response to cascades. For instance, the reconfiguration of one pure Fe twist GB suggests that GB geometry can significantly influence defect generation mechanisms. These findings point to the potential of GB engineering in developing materials with enhanced radiation tolerance, advocating for a nuanced approach to material design. By tailoring GB properties and selectively introducing dopant elements, materials can be optimized to exhibit superior resistance to radiation-induced damage, offering insights for applications in nuclear reactors and other radiation-prone environments.

cond-mat.mtrl-sci↗

arXiv2023

Stand-off runaway electron beam termination by tungsten particulates for tokamak disruption mitigation

Stand-off runaway electron termination by injected tungsten particulates offers a plausible option in the toolbox of disruption mitigation. Tungsten is an attractive material choice for this application due to large electron stopping power and high melting point. To assess the feasibility of this scheme, we simulate runaway collisions with tungsten particulates using the MCNP program for incident runaway energies ranging from 1 to 10 MeV. We assess runaway termination from energetics and collisional kinematics perspectives. Energetically, the simulations show that 99% of runaway beam energy is removed by tungsten particulates on a timescale of 4-9 $μ$s. Kinematically, the simulations show that 99% of runaways are terminated by absorption or backscattering on a timescale of 3-4 $μ$s. By either metric, the runaway beam is effectively terminated before the onset of particulate melting. Furthermore, the simulations show that secondary radiation emission by tungsten particulates does not significantly impact the runaway termination efficacy of this scheme. Secondary radiation is emitted at lower particle energies than the incident runaways and with a broad angular distribution such that the majority of secondary electrons emitted will not experience efficient runaway re-acceleration. Overall, the stand-off runaway termination scheme is a promising concept for last-ditch runaway mitigation in ITER, SPARC, and other future burning-plasma tokamaks.

physics.plasm-ph↗

arXiv2022

Machine learning in nuclear materials research

Nuclear materials are often demanded to function for extended time in extreme environments, including high radiation fluxes and transmutation, high temperature and temperature gradients, stresses, and corrosive coolants. They also have a wide range of microstructural and chemical makeup, with multifaceted and often out-of-equilibrium interactions. Machine learning (ML) is increasingly being used to tackle these complex time-dependent interactions and aid researchers in developing models and making predictions, sometimes with better accuracy than traditional modeling that focuses on one or two parameters at a time. Conventional practices of acquiring new experimental data in nuclear materials research are often slow and expensive, limiting the opportunity for data-centric ML, but new methods are changing that paradigm. Here we review high-throughput computational and experimental data approaches, especially robotic experimentation and active learning that based on Gaussian process and Bayesian optimization. We show ML examples in structural materials ( e.g., reactor pressure vessel (RPV) alloys and radiation detecting scintillating materials) and highlight new techniques of high-throughput sample preparation and characterizations, and automated radiation/environmental exposures and real-time online diagnostics. This review suggests that ML models of material constitutive relations in plasticity, damage, and even electronic and optical responses to radiation are likely to become powerful tools as they develop. Finally, we speculate on how the recent trends in artificial intelligence (AI) and machine learning will soon make the utilization of ML techniques as commonplace as the spreadsheet curve-fitting practices of today.

cond-mat.mtrl-sci↗

arXiv2017

The conundrum of relaxation volumes in first-principles calculations of charge defects

The defect relaxation volumes obtained from density-functional theory (DFT) calculations of charged vacancies and interstitials are much larger than their neutral counterparts, seemingly unphysically large. In this work, we investigate the possible reasons for this and revisit the methods that address the calculation of charged defect structures in periodic DFT. We probe the dependence of the proposed energy corrections to charged defect formation energies on relaxation volumes and find that corrections such as the image charge correction and the alignment correction, which can lead to sizable changes in defect formation energies, have an almost negligible effect on the charged defect relaxation volume. We also investigate the volume for the net neutral defect reactions comprised of individual charged defects, and find that the aggregate formation volumes have reasonable magnitudes. This work highlights an important issue that, as for defect formation energies, the defect formation volumes depend on the choice of reservoir. We show that considering the change in volume of the electron reservoir in the formation reaction of the charged defects, analogous to how volumes of atoms are accounted for in defect formation volumes, can renormalize the formation volumes of charged defects such that they are comparable to neutral defects. This approach enables the description of the elastic properties of isolated charged defects within the overall neutral material, beyond the context of the overall defect reactions that produce the charged defect.

cond-mat.mtrl-sci↗

arXiv2016

Synthesis and characterization of dense Gd2Ti2O7 pyrochlore thin films deposited using RF magnetron sputtering

Thin films of phase pure pyrochlore Gd2Ti2O7 have been synthesized by RF magnetron sputtering. The films were prepared from oxide targets in 50%O2/Ar atmosphere and deposited on 111 YSZ substrates at a temperature of 800C. The pyrochlore structure was confirmed via grazing angle x-ray diffraction and selected area electron diffraction (SAED). TEM analysis also showed that the films were dense and of uniform thickness with surface roughness of approximately 8nm. The total conductivity measured with AC impedance spectroscopy was found to be independent of thickness and comparable in magnitude to that of bulk Gd2Ti2O7. Differences were observed in the Arrhenius behavior between the bulk and thin film samples and are attributed to varying levels of background impurities.

cond-mat.mtrl-sci↗

arXiv2016

Evidence for percolation diffusion of cations and material recovery in disordered pyrochlore from accelerated molecular dynamics simulations

We used classical and accelerated molecular dynamics simulations to characterize vacancy-mediated diffusion of cations in Gd$_2$Ti$_2$O$_7$ pyrochlore as a function of the disorder on the microsecond timescale. We find that cation vacancy diffusion is slow in materials with low levels of disorder. However, higher levels of disorder allow for fast cation diffusion, which is then also accompanied by fast antisite annihilation and ordering of the cations. The cation diffusivity is therefore not constant, but decreases as the material reorders. The results suggest that fast cation diffusion is triggered by the existence of a percolation network of antisites. This is in marked contrast with oxygen diffusion, which showed a smooth increase of the ionic diffusivity with increasing disorder in the same compound. The increase of the cation diffusivity with disorder is also contrary to observations from other complex oxides and disordered media models, suggesting a fundamentally different relation between disorder and mass transport. These results highlight the dynamic interplay between fast cation diffusion and the recovery of disorder and have important implications for understanding radiation damage evolution, sintering and aging, as well as diffusion in disorder oxides more generally.

cond-mat.mtrl-sci↗

arXiv2015

Band-gap and Band-edge Engineering of Multicomponent Garnet Scintillators: A First-principles Study

Complex doping schemes in RE$_3$Al$_5$O$_{12}$ (RE=rare earth element) garnet compounds have recently led to pronounced improvements in scintillator performance. Specifically, by admixing lutetium and yttrium aluminate garnets with gallium and gadolinium, the band-gap was altered in a manner that facilitated the removal of deleterious electron trapping associated with cation antisite defects. Here, we expand upon this initial work to systematically investigate the effect of substitutional admixing on the energy levels of band edges. Density functional theory was used to survey potential admixing candidates that modify either the conduction band minimum (CBM) or valence band maximum (VBM). We considered two sets of compositions based on Lu$_3$B$_5$O$_{12}$ where B = Al, Ga, In, As, and Sb; and RE$_3$Al$_5$O$_{12}$, where RE = Lu, Gd, Dy, and Er. We found that admixing with various RE cations does not appreciably effect the band gap or band edges. In contrast, substituting Al with cations of dissimilar ionic radii has a profound impact on the band structure. We further show that certain dopants can be used to selectively modify only the CBM or the VBM. Specifically, Ga and In decrease the band gap by lowering the CBM, while As and Sb decrease the band gap by raising the VBM. These results demonstrate a powerful approach to quickly screen the impact of dopants on the electronic structure of scintillator compounds, identifying those dopants which alter the band edges in very specific ways to eliminate both electron and hole traps responsible for performance limitations. This approach should be broadly applicable for the optimization of electronic and optical performance for a wide range of compounds by tuning the VBM and CBM.

cond-mat.mtrl-sci↗

arXiv2014

Diffusion and transformation kinetics of small Helium clusters in bulk Tungsten

The production of energy through nuclear fusion poses serious challenges related to the stability and performance of materials in extreme conditions. In particular, the constant bombardment of the walls of the reactor with high doses of He ions is known to lead to deleterous changes in their microstructures. These changes follow from the aggregation of He into bubbles that can grow and blister, potentially leading to the contamination of the plasma, or to the degradation of their mechanical properties. We computationally study the behavior of small clusters of He atoms in W in conditions relevant to fusion energy production. Using a wide range of techniques, we investigate the thermodynamics of the clusters and their kinetics in terms of diffusivity, growth, and breakup, as well as mutation into nano-bubbles. Our study provides the essential ingredients to model the early stages of He exposure leading up to the nucleation of He bubbles.

cond-mat.mtrl-sci↗