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At least 919 records · Page 51

Structure and migration of heavily irradiated grain boundaries and dislocations in Ni in the athermal limit

The microstructural evolution at and near preexisting grain boundaries (GBs) and dislocations in materials under high radiation doses is still poorly understood. In this work, we use the creation relaxation algorithm (CRA) developed for atomistic modeling of high-dose irradiation in bulk materials to probe the athermal limit of saturation of GB and dislocation core regions under irradiation in fcc Ni. We find that, upon continuously subjecting a single dislocation or GB to Frenkel pair creation in the athermal limit, a local steady-state disordered defect structure is reached with excess properties that fluctuate around constant values. Case studies are given for a straight screw dislocation which elongates into a helix under irradiation and several types of low- and high-angle GBs, which exhibit coupled responses such as absorption of extrinsic dislocations, roughening, and migration. A positive correlation is found between the initial GB energy and the local steady-state GB energy under irradiation across a wide variety of GB types. Metastable GB structures with similar density in the defect core region but different initial configurations are found to converge to the same limiting structure under CRA. The mechanical responses of pristine and irradiated dislocations and GB structures are compared under an applied shear stress. Irradiated screw and edge dislocations are found to exhibit a hardening response, migrating at larger flow stresses than their pristine counterparts. Mobile GBs are found to exhibit softening or hardening responses depending on GB character. Although some GBs recover their initial pristine structures upon migration outside of the radiation zone, many GBs sustain different flow stresses corresponding to altered mobile core structures.

36 MATERIALS SCIENCE↗

Rapid Initial-State Preparation for the Quantum Simulation of Strongly Correlated Molecules

Studies on quantum algorithms for ground-state energy estimation often assume perfect ground-state preparation; however, in reality the initial state will have imperfect overlap with the true ground state. Here, we address that problem in two ways: by faster preparation of matrix-product-state (MPS) approximations and by more efficient filtering of the prepared state to find the ground-state energy. We show how to achieve unitary synthesis with a Toffoli complexity about 7 × lower than that in prior work and use that to derive a more efficient MPS-preparation method. For filtering, we present two different approaches: sampling and binary search. For both, we use the theory of window functions to avoid large phase errors and minimize the complexity. We find that the binary-search approach provides better scaling with the overlap at the cost of a larger constant factor, such that it will be preferred for overlaps less than about 0.003 . Finally, we estimate the total resources to perform ground-state energy estimation of Fe - S cluster systems, including the Fe Mo cofactor by estimating the overlap of different MPS initial states with potential ground states of the Fe Mo cofactor using an extrapolation procedure. With a modest MPS bond dimension of 4000 , our procedure produces an estimate of approximately 0.9 overlap squared with a candidate ground state of the Fe Mo cofactor, producing a total resource estimate of 7.3 × 10 10 Toffoli gates; neglecting the search over candidates and assuming the accuracy of the extrapolation, this validates prior estimates that have used perfect ground-state overlap. This presents an example of a practical path to prepare states of high overlap in a challenging-to-compute chemical system. Published by the American Physical Society 2025

Berry, Dominic W. (ORCID:0000000334461449)↗

Conditional diffusion machine-learning framework for mapping valence electron distribution from convergent beam electron diffraction

Quantitative convergent beam electron diffraction (CBED) enables determination of aspherical valence electron distributions through refinement of low-order structure factors, which are highly sensitive to chemical bonding and charge density variations. However, conventional quantitative CBED (QCBED) requires solving a highly nonlinear inverse problem with many coupled parameters, and computationally intensive dynamical diffraction calculations, making it time-consuming and difficult to apply to complex systems. More broadly, reconstructing charge density and orbital electron distribution from diffraction data has long been a central challenge in both x-ray and electron crystallography. Here, in this study, we introduce an artificial-intelligence (AI)-based framework that replaces traditional refinement with a data-driven inverse solver. Using a large synthetic CBED dataset generated by Bloch-wave simulations, we train a conditional diffusion model to directly infer crystal structural parameters and multipole density formalism parameters, and hence valence electron distributions, from CBED patterns alone. By learning from forward simulations across realistic parameter space, the model effectively solves the inverse problem. Compared with direct regression approaches, the diffusion-based framework provides posterior parameter distributions for rigorous uncertainty quantification while preserving quantitative fidelity and reducing analysis time by orders of magnitude. By eliminating the need for external single-crystal x-ray diffraction data and complex nonlinear refinement, this approach enables practical, high-throughput, and in situ quantitative CBED, enabling real-time mapping of valence electron distributions and their correlation with functional responses in quantum and energy materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Lanczos algorithm for lattice QCD matrix elements

Recent work [M. L. Wagman, Lanczos, the transfer matrix, and the signal-to-noise problem, .] found that an analysis formalism based on the Lanczos algorithm allows energy levels to be extracted from Euclidean correlation functions with faster ground-state convergence than effective masses, convergent estimators for multiple states from a single correlator, and two-sided error bounds. After filtering out spurious eigenvalues and using outlier-robust estimators within a nested bootstrap framework, Lanczos estimators behave more like multistate fit results than effective masses—but without involving statistical fitting. We extend this formalism to the determination of matrix elements from three-point correlation functions and provide a physical picture of “spurious-state filtering” involving restriction to a Hermitian subspace. We demonstrate similar advantages for matrix elements as for spectroscopy through example applications to noiseless mock-data and (bare) forward matrix elements of the strange scalar current between both ground and excited states with the quantum numbers of the nucleon.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Ion beam irradiation of ABO4 compounds with the fergusonite, monazite, scheelite, and zircon structures

The effects of irradiation on CaWO4, SrWO4, BaWO4, YVO4, LaVO4, YNbO4, and LaNbO4 were investigated on thin crystals using 1.0 MeV Kr ions at 50-1000 K. All of the ABO4 compounds can be amorphized with calculated damage cross sections (σa = 1/Fc0) in the range of ~0.30-1.09 × 10-14 cm2 ion-1 at zero Kelvin. The analysis of fluence-temperature data returned critical temperatures for amorphization (Tc) of 311 ± 1, 358 ± 90, 325 ± 19, 415 ± 17, 541 ± 6, 636 ± 26, and 1012 ± 1 K, respectively, for the compounds listed above. Compared with previous in situ irradiation of ABO4 orthophosphate samples using 0.8 MeV Kr ions, the Tc values of LaVO4 and YVO4 are higher than those of LaPO4 and YPO4 by 82 K and 124 K, respectively. The Tc values of the three scheelite structures, CaWO4, SrWO4, and BaWO4, indicate that they are the most radiation tolerant compounds under these conditions. The A-B cation anti-site energies, EfAB, determined by DFT range from 2.48 to 10.58 eV and are highly correlated with the A-B cation ionic radius ratio, rA/rB, but are not correlated with Tc across the different structure types, suggesting that the formation and migration energies of Frenkel defects play a more important role in damage recovery in these compounds. We also discuss the role of cation and anion charge/iconicity as determined by DFT. ABO4 compounds with the zircon structure and B = P or V have a distinct advantage over those with B = Si as the damaged regions do not appear to be significantly affected by polymerization of (PO4) 3- or (VO4) 3- groups which might stabilize the amorphous fraction and ultimately lead to phase separation as observed in zircon (ZrSiO4).

amorphization↗

A Micro-Mechanical Constitutive Model to Predict Hygrothermal Aging of Cross-Linked Polymers

Abstract A multi-physics material model is presented to describe the effects of temperature, oxygen, and humidity on the constitutive response of cross-linked polymers. The effect of hygrothermal damage on the mechanical integrity of the polymer matrix can be considered as the result of damage accumulation of two independent aging mechanism namely, i) thermo-oxidative, and ii) hydrolytic aging. In order to capture the mutual effects of thermo-oxidative and hydrolytic aging, an assumption has been made that each of the aging phenomenon can be superposed to each other. In fact, each of them works independently and as a result, they can compete with each other. Utilizing the theory of network decomposition, all phenomena and their correlation were modeled and thus, the strain energy function of the polymer matrix is written with respect to four independent mechanisms, i) the shrinking original matrix that has neither been attacked by water nor oxygen, ii) conversion of the first network to two new network due to the reduction and formation of cross-links, and iii) energy loss from network degradation due to attack of the water molecules to polymer active agents. Moreover, the proposed model is micro-mechanically based and is mainly relevant on thin samples due to our underlying assumption of homogeneous diffusion of oxygen and water throughout the matrix. The model has been validated against extensive data-sets obtained from experiments we specifically designed for concept validation.

Bahrololoumi, Amir↗

Vibronic and Environmental Effects in Simulations of Optical Spectroscopy

Including both environmental and vibronic effects is important for accurate simulation of optical spectra, but combining these effects remains computationally challenging. We outline two approaches that consider both the explicit atomistic environment and the vibronic transitions. Both phenomena are responsible for spectral shapes in linear spectroscopy and the electronic evolution measured in nonlinear spectroscopy. The first approach utilizes snapshots of chromophore-environment configurations for which chromophore normal modes are determined. We outline various approximations for this static approach that assumes harmonic potentials and ignores dynamic system-environment coupling. The second approach obtains excitation energies for a series of time-correlated snapshots. This dynamic approach relies on the accurate truncation of the cumulant expansion but treats the dynamics of the chromophore and the environment on equal footing. Both approaches show significant potential for making strides toward more accurate optical spectroscopy simulations of complex condensed phase systems.

Chemistry↗

Multi-Trait Regressor Stacking Increased Genomic Prediction Accuracy of Sorghum Grain Composition

Genomic prediction has enabled plant breeders to estimate breeding values of unobserved genotypes and environments. The use of genomic prediction will be extremely valuable for compositional traits for which phenotyping is labor-intensive and destructive for most accurate results. We studied the potential of Bayesian multi-output regressor stacking (BMORS) model in improving prediction performance over single trait single environment (STSE) models using a grain sorghum diversity panel (GSDP) and a biparental recombinant inbred lines (RILs) population. A total of five highly correlated grain composition traits—amylose, fat, gross energy, protein and starch, with genomic heritability ranging from 0.24 to 0.59 in the GSDP and 0.69 to 0.83 in the RILs were studied. Average prediction accuracies from the STSE model were within a range of 0.4 to 0.6 for all traits across both populations except amylose (0.25) in the GSDP. Prediction accuracy for BMORS increased by 41% and 32% on average over STSE in the GSDP and RILs, respectively. Prediction of whole environments by training with remaining environments in BMORS resulted in moderate to high prediction accuracy. Our results show regression stacking methods such as BMORS have potential to accurately predict unobserved individuals and environments, and implementation of such models can accelerate genetic gain.

54 ENVIRONMENTAL SCIENCES↗

Ab Initio Study of the Effect of Mono-Vacancies on the Metastability of Ga-Stabilized δ-Pu

Most experimental studies on metallic Pu are on the room temperature monoclinic α-phase or the fcc Ga stabilized δ-phase. Stabilized δ-phase Pu-Ga alloys are metastable and exhibit a martensitic phase transformation to α’-phase at low temperatures, or applied shear, with concentrations lower than three atomic percent Ga. By using first principles, we explore the metastability of δ-phase by investigating the structural and electronic behavior induced by Ga alloying and by a mono-vacancy point defect. We find that a site substitutional Ga induces a tetragonal distortion in the lattice affected by hybridization of Ga 4p and Pu 6d states. With the addition of a mono-vacancy, a monoclinic or tetragonal distortion forms locally (dependent on its distance from Ga), and decoupling of the Pu 5f and 6d states and broadening of the 6d states occurs. This response enables hybridization of Pu 6d with the Ga 4p states affecting the mono-vacancy formation energy. Thus, stabilization of the fcc lattice correlates with hybridization of Pu 6d states with Ga 4p states, and this becomes more evident in the presence of a mono-vacancy.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Photometric Analyses of Saturn’s Small Moons: Aegaeon, Methone, and Pallene Are Dark; Helene and Calypso Are Bright

We examine the surface brightnesses of Saturn’s smaller satellites using a photometric model that explicitly accounts for their elongated shapes and thus facilitates comparisons among different moons. Analyses of Cassini imaging data with this model reveal that the moons Aegaeon, Methone, and Pallene are darker than one would expect given trends previously observed among the nearby mid-sized satellites. On the other hand, the trojan moons Calypso and Helene have substantially brighter surfaces than their co-orbital companions Tethys and Dione. These observations are inconsistent with the moons’ surface brightnesses being entirely controlled by the local flux of E-ring particles, and therefore strongly imply that other phenomena are affecting their surface properties. The darkness of Aegaeon, Methone, and Pallene is correlated with the fluxes of high-energy protons, implying that high-energy radiation is responsible for darkening these small moons. Meanwhile, Prometheus and Pandora appear to be brightened by their interactions with the nearby dusty F ring, implying that enhanced dust fluxes are most likely responsible for Calypso’s and Helene’s excess brightness. However, there are no obvious structures in the E ring that would preferentially brighten these two moons, so there must either be something subtle in the E-ring particles’ orbital properties that leads to asymmetries in the relevant fluxes, or something happened recently to temporarily increase these moons’ brightnesses.

79 ASTRONOMY AND ASTROPHYSICS↗

EGR Dilution and Fuel Property Effects on High-Efficiency Spark-Ignition Flames

Modern spark ignition internal combustion engines rely on fast combustion rates and high dilution to achieve high brake thermal efficiencies. To accomplish this, new engine designs have moved towards increased tumble ratios and stroke-to-bore ratios. Increased tumble ratios correlate positively with increases in turbulent kinetic energy and improved fuel and residual gas mixing, all of which favor faster and more efficient combustion. Longer stroke-to-bore ratios allow higher geometric compression ratios and use of late intake valve closing to control peak compression pressures and temperatures. The addition of dilution to improve efficiency is limited by the resulting increase in combustion instabilities manifested by cycle-to-cycle variability. A number of effects - preferential diffusion, turbulence-combustion interactions, stochastic flow patterns, laminar-turbulent flame kernel transitions, and relative length and velocity scales between flame and turbulence - are believed to be responsible for the increase in cycle-to-cycle variations, where their contributions are likely interlinked. Several studies have shown the influence of stochastic flow characteristics on the nature of combustion instabilities, such as velocity patterns on flame kernel formation and cycle-to-cycle variations in residual gas. However, few have focused on the specific effects of fuel properties. The objective of this work is to contrast the effects of dilution on propane stoichiometric combustion against gasoline. Dilution tolerance experiments were conducted in a purpose-built high stroke-to-bore ratio single cylinder engine with both gasoline and LPG. Three-dimensional full cycle computational fluid dynamics (CFD) simulations employing a level-set combustion approach and Reynolds averaged Navier-Stokes (RANS) turbulence modeling was used to qualitatively assess the changes in length and velocity scales for turbulence and the flame. The experimental results showed that LPG can tolerate higher exhaust gas recirculation (EGR) dilution under a variety of conditions. Analysis of CFD simulations showed that propane flames are likely less sensitive to influences from the flow field due to less thickening of the flame and higher effective flame speeds.

33 ADVANCED PROPULSION SYSTEMS↗

OC6 project Phase IV: validation of numerical models for novel floating offshore wind support structures

Abstract. This paper provides a summary of the work done within Phase IV of the Offshore Code Comparison Collaboration, Continued with Correlation and unCertainty (OC6) project, under International Energy Agency Wind Technology Collaboration Programme Task 30. This phase focused on validating the loading on and motion of a novel floating offshore wind system. Numerical models of a 3.6 MW horizontal-axis wind turbine atop the TetraSpar floating support structure were compared using measurement data from a 1:43-Froude-scale test performed in the University of Maine's Alfond Wind–Wave (W2) Ocean Engineering Laboratory. Participants in the project ran a series of simulations, including system equilibrium, surge offsets, free-decay tests, wind-only conditions, wave-only conditions, and a combination of wind and wave conditions. Validation of the models was performed by comparing the aerodynamic loading, floating support structure motion, tower base loading, mooring line tensions, and keel line tensions. The results show a relatively good estimation of the aerodynamic loading and a reasonable estimation of the platform motion and tower base fore–aft bending moment. However, there is a significant dispersion in the dynamic loading for the upwind mooring line. Very good agreement was observed between most of the numerical models and the experiment for the keel line tensions.

17 WIND ENERGY↗

First characterization of the emission behavior of Mrk 421 from radio to very high-energy gamma rays with simultaneous X-ray polarization measurements

Aims.We have performed the first broadband study of Mrk 421 from radio to TeV gamma rays with simultaneous measurements of the X-ray polarization from IXPE. Methods.The data were collected as part of an extensive multiwavelength campaign carried out between May and June 2022 using MAGIC,Fermi-LAT,NuSTAR,XMM-Newton,Swift, and several optical and radio telescopes to complement IXPE data. Results.During the IXPE exposures, the measured 0.2–1 TeV flux was close to the quiescent state and ranged from 25% to 50% of the Crab Nebula without intra-night variability. Throughout the campaign, the very high-energy (VHE) and X-ray emission are positively correlated at a 4σsignificance level. The IXPE measurements reveal an X-ray polarization degree that is a factor of 2–5 higher than in the optical/radio bands; that implies an energy-stratified jet in which the VHE photons are emitted co-spatially with the X-rays, in the vicinity of a shock front. The June 2022 observations exhibit a rotation of the X-ray polarization angle. Despite no simultaneous VHE coverage being available during a large fraction of the swing, theSwift-XRT monitoring reveals an X-ray flux increase with a clear spectral hardening. This suggests that flares in high synchrotron peaked blazars can be accompanied by a polarization angle rotation, as observed in some flat spectrum radio quasars. Finally, during the polarization angle rotation,NuSTARdata reveal two contiguous spectral hysteresis loops in opposite directions (clockwise and counterclockwise), implying important changes in the particle acceleration efficiency on approximately hour timescales.

Astronomy & Astrophysics↗

Elucidation of Marcus Relationships for Hydride Transfer Reactions Involving Transition Metal Hydrides

The rate of hydride transfer from three Ir hydride complexes of the type Cp*Ir( R bpy)H + (Cp* = C 5 Me 5 ; R bpy = 4,4′-R-2,2′-bipyridine, R = OMe, H, CO 2 Me) to six N-methylacridinium ( R Acr + ) acceptors with electronically different substituents in the 2- or 2,7-positions were measured. Using the thermodynamic hydricity of the donors and the hydride affinity of the acceptors the thermodynamic driving forces for hydride transfer were determined. Brønsted plots, which correlate kinetic and thermodynamic hydricity, demonstrate distinct linear free energy relationships for each complex, with different Brønsted α values. Thus, at the same driving force hydride transfer from Cp*Ir( OMe bpy)H + is faster than for Cp*Ir(bpy)H + or Cp*Ir( CO2Me bpy)H + . Experimental and computational analyses are consistent with a concerted hydride transfer mechanism for all Ir complexes. As the thermodynamic driving force increases an earlier transition state is observed and all transition states also include π-stacking interactions between the donor and acceptor, which likely contribute to the different α values. The experimental data fits well to the Marcus model, enabling the determination of reorganization energies (λ) that range from 58 to 69 kcal mol -1 . These are lower than λ values for hydride transfer reactions involving organic donors and acceptors. This work provides a rare example of the correlation of kinetic and thermodynamic hydricity using only experimental data and shows that hydride transfer reactions involving metal hydrides can follow Marcus theory. Furthermore, the findings offer insight into controlling metal-catalyzed hydride transfer reactions, which is valuable for designing improved systems for a range of transformations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The effect of selection – a tale of cluster mass measurement bias induced by correlation and projection

ABSTRACT Cosmology analyses using galaxy clusters by the Dark Energy Survey have recently uncovered an issue of a previously unknown selection effect affecting weak-lensing mass estimates. In this letter, we use the Illustris-TNG simulation to demonstrate that selecting on galaxy counts induces a selection effect because of projection and correlation between different observables. We compute the weak-lensing-like projected mass estimations of dark matter haloes and examine their projected subhalo counts. In the two-dimensional (2D) projected space, haloes that are measured as more massive than truth have higher subhalo counts. Thus, projection along the line of sight creates cluster observables that are correlated with cluster mass measurement deviations, which in turn creates a mass measurement bias when the clusters are selected by this correlated observable. We demonstrate that the bias is predicted in a forward model using the observable-mass measurement correlation.

79 ASTRONOMY AND ASTROPHYSICS↗

Comparative study of Minnesota functionals performance on ferroelectric BaTiO 3 and PbTiO 3

Density functional theory based simulations are the leading tool for the computational investigation of ferroelectrics and the parametrization of their classical potentials. However, the predictions often depend strongly on the exchange correlation functional. The most popular choices, LDA and GGA, tend to underestimate or overestimate some structural, electric, and energy properties. These impede development of highly accurate classical potentials that extend the reach of first-principles simulations to finite temperatures and realistic sizes. In this work, we investigate the performance of recently developed Minnesota exchange correlation functionals on prototypical ferroelectrics BaTiO 3 , and PbTiO 3 , in comparison with some popular ones. We find that there exists strong correlation between predictions for some properties (tetragonality, phase energy difference, and polarization) by different functionals. Along the correlation line, we find a range of functionals (including some from the Minnesota suite) whose predictions fall in between those of LDA and GGA and, therefore, offer an improvement. A way to relatively rank functional performance with respect to chosen benchmarks is proposed and applied to identify the top performers for BaTiO 3 and PbTiO 3 . Here, the performance is found to be material dependent. Therefore, we propose that the performance assessment carried out in this work is employed to "screen" functionals prior to their use on ferroelectrics. Quick and computationally inexpensive, it is likely to lead to improved descriptions, especially for classical potential parametrization. The Minnesota functional suite is found to be suitable for this task.

36 MATERIALS SCIENCE↗

Generation and validation of comprehensive synthetic weather histories using auto-regressive moving-average models

As energy system design moves to more complex methods of optimization including machine learning there is a significant need for more weather data than is available. One method to solve this is using synthetic data models such as the auto-regressive moving-average (ARMA) model which has been frequently utilized to create such data. This paper looks at extending the ARMA algorithm to generate solar components through the use of clearsky detrending, maintaining vector relationships and by leveraging physical relationships. The method for the creation of entirely synthetic weather data files including key weather variables for energy system analysis is presented. Furthermore, a detailed comparison of energy system simulations utilizing both real and synthetic data is made using NREL’s System Advisor Model. Whilst good agreement is made for the solar variables, and other weather variables, ARMA methods often fail to capture the standard deviation and skew of annual weather distributions. Vector-ARMA is shown to maintain correlations between variables and thus generate data sets that perform similarly in energy system design. Here, it is finally shown that the ARMA method fails to preserve day-today correlations in weather variables and thus over-predicts optimal energy storage by 21% for a residential solar application.

42 ENGINEERING↗

Multiscale Physics of Atomic Nuclei from First Principles

Atomic nuclei exhibit multiple energy scales ranging from hundreds of MeV in binding energies to fractions of an MeV for low-lying collective excitations. As the limits of nuclear binding are approached near the neutron and proton drip lines, traditional shell structure starts to melt with an onset of deformation and an emergence of coexisting shapes. It is a long-standing challenge to describe this multiscale physics starting from nuclear forces with roots in quantum chromodynamics. Here, we achieve this within a unified and nonperturbative quantum many-body framework that captures both short- and long-range correlations starting from modern nucleon-nucleon and three-nucleon forces from chiral effective field theory. The short-range (dynamic) correlations which account for the bulk of the binding energy are included within a symmetry-breaking framework, while long-range (static) correlations (and fine details about the collective structure) are included by employing symmetry projection techniques. Our calculations accurately reproduce—within theoretical error bars—available experimental data for low-lying collective states and the electromagnetic quadrupole transitions in 20−30 Ne. In addition, we reveal coexisting spherical and deformed shapes in 30 Ne, which indicates the breakdown of the magic neutron number 𝑁 = 20 as the key nucleus 28 O is approached, and we predict that the drip line nuclei 32,34 Ne are strongly deformed and collective. By developing reduced-order models for symmetry-projected states, we perform a global sensitivity analysis and find that the subleading singlet 𝑆-wave contact and a pion-nucleon coupling strongly impact nuclear deformation in chiral effective field theory. The techniques developed in this work clarify how microscopic nuclear forces generate the multiscale physics of nuclei spanning collective phenomena as well as short-range correlations and allow one to capture emergent and dynamical phenomena in finite fermion systems such as atom clusters, molecules, and atomic nuclei.

74 ATOMIC AND MOLECULAR PHYSICS↗