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At least 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Preface to the JPCM special issue on intense radiation sources in condensed matter and materials physics

This special issue is designed to honour the contributions of our colleague Neville Greaves who was among the first to apply newly-available synchrotron x-ray techniques to study the synthesis, structures and properties of advanced materials [1, 2]. His wide ranging work on ceramics, glasses and nanomaterials was celebrated in a recent issue of the J. Non-Cryst. Solids [3]. Neville's contributions to synchrotron research, highlighted here, focussed on design and construction of new beamline capabilities and sample environments to probe materials under different physical and chemical conditions, integrating various techniques to obtain complementary data on structure and bonding. The innovative nature of his work is illustrated by his studies of liquids and glasses, where he incorporated aerodynamic levitation into these experimental techniques, using both synchrotron x-ray and neutron beams to probe the structural transformations and dynamics combined with molecular dynamics simulations to study atomic scale organisation. His work has had a major impact on fundamental condensed matter physics and chemistry as well as applied materials science; and in this issue, we present contributions from colleagues using and developing new experimental techniques at current and next-generation synchrotron, neutron and free-electron laser sources and in their own laboratories, that probe the fundamental physics, chemistry and functional properties of novel materials and processes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Interpreting nanovoids in atom probe tomography data for accurate local compositional measurements

Quantifying chemical compositions around nanovoids is a fundamental task for research and development of various materials. Atom probe tomography (APT) and scanning transmission electron microscopy (STEM) are currently the most suitable tools because of their ability to probe materials at the nanoscale. Both techniques have limitations, particularly APT, because of insufficient understanding of void imaging. Here, we employ a correlative APT and STEM approach to investigate the APT imaging process and reveal that voids can lead to either an increase or a decrease in local atomic densities in the APT reconstruction. Simulated APT experiments demonstrate the local density variations near voids are controlled by the unique ring structures as voids open and the different evaporation fields of the surrounding atoms. We provide a general approach for quantifying chemical segregations near voids within an APT dataset, in which the composition can be directly determined with a higher accuracy than STEM-based techniques.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Precise Modulation of CO 2 Sorption in Ti 8 Ce 2 –Oxo Clusters: Elucidating Lewis Acidity of the Ce Metal Sites and Structural Flexibility

Investigating the structure-property correlation in porous materials is a fundamental and consistent focus in various scientific domains, especially within sorption research. Metal oxide clusters with capping ligands, characterized by intrinsic cavities formed through specific solid-state packing, demonstrate significant potential as versatile platforms for sorption investigations due to their precisely tunable atomic structures and inherent long-range order. This study presents a series of Ti 8 Ce 2 -oxo clusters with subtle variations in coordinated linkers and explores their sorption behavior. Notably, Ti 8 Ce 2 -BA (BA denotes benzoic acid) manifests a distinctive two-step profile during CO 2 adsorption, accompanied by a hysteresis loop. This observation marks a new instance within the metal oxide cluster field. Of intrigue, the presence of unsaturated Ce(IV) sites was found to be correlated with the stepped sorption property. Moreover, the introduction of an electrophilic fluorine atom, positioned ortho or para to the benzoic acid, facilitated precise control over gate pressure and stepped sorption quantities. Advanced in-situ techniques systematically unraveled the underlying mechanism behind this unique sorption behavior. The findings elucidate that robust Lewis base-acid interactions are established between CO 2 molecules and Ce ions, consequently altering the conformation of coordinated linkers. Conversely, the F atoms primarily contribute to gate pressure variation by influencing the Lewis acidity of the Ce sites. This research advances the understanding in fabricating metal-oxo clusters with structural flexibility and provides profound insights into their host-guest interaction motifs. Furthermore, these insights hold substantial promise across diverse fields and offer valuable guidance for future adsorbent designs grounded in fundamental theories of structure-property relationships.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Atom Interferometry with Floquet Atom Optics

Floquet engineering offers a compelling approach for designing the time evolution of periodically driven systems. We implement a periodic atom-light coupling to realize Floquet atom optics on the strontium 1 S 0 - 3 P 1 transition. These atom optics reach pulse efficiencies above 99.4% over a wide range of frequency offsets between light and atomic resonance, even under strong driving where this detuning is on the order of the Rabi frequency. Moreover, we use Floquet atom optics to compensate for differential Doppler shifts in large momentum transfer atom interferometers and achieve state-of-the-art momentum separation in excess of 400 ℏ⁢k. In conclusion, this technique can be applied to any two-level system at arbitrary coupling strength, with broad application in coherent quantum control.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Short-range order and longer-range disorder revealed in germanium–tin alloy thin films by extended x-ray absorption fine structure analysis

Short-range order (SRO) in semiconductor alloys, a relatively under-studied structural phenomenon in which local atomic arrangements differ from those of a random solid solution, is investigated in molecular beam epitaxy (MBE)-grown GeSn thin films. A novel preparation technique is used to pattern these films into microscale ribbons that are released from the substrate for extended x-ray absorption fine structure (EXAFS) analysis. The results indicate a strong SRO in which the first shell around Sn atoms is greatly denuded of Sn atoms relative to the nominal atomic composition of the alloy. This effect is more pronounced than that observed recently in GeSn nanowires grown by chemical vapor deposition. Additionally, the presence of a longer-range disorder detected by EXAFS analysis in the shells of atoms more distant from the absorbers is indicative of the defects and inhomogeneous strain present in the MBE-grown films. The evident existence of the SRO in GeSn alloys deposited by different growth methods and in different strain states suggests that SRO is a general phenomenon in the thin films of this metastable solid solution.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Laser interference structuring of Cu for adhesive joining of HVAC equipment

Due to potential energy and cost savings benefits, adhesive joining has been recently considered for heating, ventilation, air conditioning, and refrigeration (HVAC&R) systems. HVAC adhesive bonding requires cost-effective and adequate surface preparations of adherents. Here, this article investigates the use of abrasion, traditional single-beam laser, and a laser-interference technique as surface preparations of copper surfaces. Surface morphology is characterized using scanning electron microscopy (SEM) and atomic force microscopy (AFM). Effective submicrometer peak-to-valley structuring with a periodicity of ∼2.7μ⁢m was demonstrated for laser-interference processing. Single-lap shear tests were conducted for 89 joints made with bondline thicknesses of 0.15 and 0.3 mm. Data on process variables and measured variables included open-time, bond length, maximum load, displacement at failure, shear lap strength, and failure mode. A statistical analysis was conducted on each lot to determine the lower limit with 95% confidence intervals for displacements at failure and shear lap strengths. A comparison is presented between the properties of laser-structured joints with respect to those prepared by abrasion, which is considered the baseline surface preparation technique. Based on this comparison, one single-beam laser technique and two laser-interference techniques were shown to exhibit vastly superior performance over the joints made with abraded specimens.

Sabau, Adrian S. [Oak Ridge National Laboratory (O↗
DOE OSTI2026

Surface Reordering During Layer‐by‐Layer Growth on SrTiO 3

With the development of layer‐by‐layer growth techniques such as molecular beam epitaxy (MBE), it is now possible to construct materials with atomic‐level precision, with the layer sequence primarily determined by the growth recipe. However, materials can still restructure in the high‐temperature growth environment with surface thermodynamics strongly influencing growth behavior. Here, we demonstrate that growth on ${\rm SrTiO}_{3}$ (001), the principal platform for oxide electronics, does not occur in a layer‐by‐layer fashion but follows a more complex process in which a ${\rm TiO}_{2}$ plane continually diffuses toward the growth surface. Employing in situ synchrotron X‐ray scattering combined with ab initio thermodynamic calculations, we discover the existence of a stable ${\rm TiO}_{2}$ double‐layer structure on the pristine substrate and the occurrence of dynamic layer rearrangement during homoepitaxial growth by oxide MBE. Our findings suggest that the current methods used to precisely control ${\rm SrTiO}_{3}$ surfaces are limited, as well as our ability to dictate the composition of ultrathin films, resulting in important ramifications regarding the surface reactivity of perovskite materials grown on ${\rm SrTiO}_{3}$.

Coherent Bragg Rod Analysis↗
DOE OSTI2025

Grain Boundary Segregation Suppresses Local Short‐Range Ordering in Nanocrystalline High‐Entropy Alloys

Multi-principal-element alloys like high-entropy alloys (HEAs) have potential applications in many engineering fields due to their unique mechanical/functional properties. While HEAs are generally considered random solid solutions, recent studies revealed that they are prone to short-range-ordering (SRO) due to the complex multi-pair-wise interactions among the constituent elements. Meanwhile, SROs' evolution can sometimes be deleterious, and it is necessary to have control over their evolution. Examining the AlCoCrFe-Zr model alloy, long-range ordering occurs following the expectation of enthalpic predictions. Advanced characterization techniques—transmission electron microscopy, high-energy synchrotron X-ray diffraction/pair distribution function, and atom probe tomography, reveal that SRO is suppressed in as-milled and GB-decorated NC-(AlCoCrFe)100-xZrx (x = 0–1.5 atomic %). Warren-Cowley coefficient calculations are further used to validate the suppression of SRO. Besides the low segregation enthalpies of Cr, Fe, and Zr, and the high-mixing enthalpy of Cr and Fe, the short diffusion path to GBs due to high-GB density in the NC-HEAs and the higher energy state of the GBs than the matrix promotes GB-segregation that further alters the matrix chemistry and consequently disfavors SRO formation within the matrix. Despite the GB-segregation of Cr, Fe, and Zr, the matrices and GBs remain in a random solid solution.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Accelerated screening of functional atomic impurities in halide perovskites using high-throughput computations and machine learning

The pressing need for novel materials that can serve rising demands in solar cell and optoelectronic technologies makes the nexus of halide perovskites, high-throughput computations, and machine learning, very promising. Ever increasing amounts of data on the structure, fundamental properties, and device performance of halide perovskites provide opportunities for learning chemical rules and design principles that make these materials attractive, and applying them across wide chemical spaces. In this work, we show that impurity properties of halide perovskites computed using density functional theory (DFT) can be combined with machine learning (ML) to deliver predictive models and quick identification of optoelectronically active impurity atoms. Our computation lead to the largest reported dataset of the formation energies and charge transition levels of Pb-site impurities in methylammonium lead halide (MAPbX 3 ) perovskites. Descriptors are defined to uniquely represent any impurity atom in any MAPbX 3 compound and mapped to the computed impurity properties using regression techniques such as Gaussian process regression, neural networks, and random forests. We use the best optimized predictive models to make predictions for hundreds of impurities across 9 MAPbX 3 compounds and create lists of dominating impurities, that is, impurities that can shift the equilibrium Fermi level in the perovskite as determined by native point defects. Finally, this accelerated screening powered by computations and machine learning can guide the identification of problematic impurities that may cause undesired recombination of charge carriers, as well as impurities that can be deliberately introduced to tune the perovskite conductivity and resulting photovoltaic absorption.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Crystal structure and magnetic properties of Gd 8 Mn 3 Sb 19

Here, in this study, a novel magnetic semimetal compound, Gd 8 Mn 3 Sb 19 , was synthesized successfully via high-temperature solid-state reaction. The crystal structure of Gd 8 Mn 3 Sb 19 was determined using both single crystal and powder X-ray diffraction techniques, revealing a non-centrosymmetric orthorhombic space group, Pmn2 1 (No. 31). The Sb atoms in Gd 8 Mn 3 Sb 19 form five-atom-wide Sb 5 7− ribbons, narrower three-atom-wide Sb 3 5− ribbons, and single Sb 3− anions. On the other hand, both Gd 3+ and Mn 2+ ions form the distorted Gd 3 and Mn 3 triangular lattices, respectively. The magnetic measurements suggest the complex magnetic interactions contributed by both Gd 3+ and Mn 2+ ions. A sharp peak observed in the magnetic susceptibility plot at approximately 25 K corresponds to the antiferromagnetic-type transition in Gd 8 Mn 3 Sb 19 . Furthermore, the magnetic measurements along different directions indicate the strong magnetic anisotropy present in Gd 8 Mn 3 Sb 19 , which is likely due to the complex magnetic interactions arising from the existence of Gd and Mn ions. Finally, the electrical resistivity measurements of Gd 8 Mn 3 Sb 19 indicate semimetallic behavior with a positive magnetoresistance.

Chemistry↗
DOE OSTI2020

Examining the multi-scale complexity and the crystallographic hierarchy of isothermally treated bainitic and martensitic structures

In this work, differences and similarities between bainitic and martensitic structures obtained by isothermal heat treatments such as austempering, quench and partitioning (Q&P) and quench and tempering (Q&T), are investigated by multiple techniques including X-ray diffraction, electron backscatter diffraction, scanning and transmission electron microscopy and atom probe tomography. Additionally, results reveal that analogous lath-like ferritic structures with similar austenite content can be achieved by adjusting the isothermal holding temperature. However, certain variability in hardness is recorded, which is consistent with differences on the precipitation state revealed by the nano-scale examination of the structure, and with dissimilar crystallographic size distribution of ferritic grains.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Molecular Picture of the Transient Nature of Lipid Rafts

In biological membranes, lipid rafts are now thought to be transient and nanoscopic. However, the mechanism responsible for these nanoscopic assemblies remains poorly understood, even in the case of model membranes. Therefore, it has proven extremely challenging to probe the physicochemical properties of lipid rafts at the molecular level. Here, we use all-atom molecular dynamics (MD) simulations and inelastic X-ray scattering (IXS), an intrinsically nanoscale technique, to directly probe the energy transfer and collective short-wavelength dynamics (phonons) of biologically relevant model membranes. We show that the nanoscale propagation of stress in lipid rafts takes place in the form of collective motions made up of longitudinal (compression waves) and transverse (shear waves) molecular vibrations. Importantly, we provide a molecular picture for the so-called van der Waals mediated "force from lipid" [Anishkin, A. et al. Proc. Natl. Acad. Sci. U.S.A. 2014, 111, 7898], a key parameter for the ionic channel mechano-transduction and the mechanism for the lipid transfer of molecular level stress [Aponte-Santamaría, C. et al. J. Am. Chem. Soc. 2017, 139, 13588]. Specifically, we describe how lipid rafts are formed and maintained through the propagation of molecular stress, lipid raft rattling dynamics, and a relaxation process. Eventually, the rafts dissipate through the self-diffusion of lipids making up the rafts. We also show that the molecular stress and viscoelastic properties of transient lipid rafts can be modulated through the use of hydrophobic biomolecules such as melatonin and tryptophan. Overall, the herein proposed mechanism describing the molecular interactions for the formation and dissolution of lipid rafts may offer insights as to how lipid rafts enable biological function.

36 MATERIALS SCIENCE↗
DOE OSTI2024

First-Principles Insights into the Thermodynamics of Variable-Temperature Ammonia Synthesis on Transition-Metal-Doped Cu (100) and (111)

Ammonia (NH 3 ) is one of the most produced chemicals worldwide. NH 3 synthesis predominantly utilizes the Haber–Bosch (HB) process, requiring high temperatures and pressures. Despite significant process advances, ample opportunity remains for improving the rate, selectivity, catalyst stability, and energy efficiency. Inspired by a recently developed programmable heating and quenching (PHQ) technique, we present in this paper a first-principles screening of candidate single-atom alloy catalysts generated from doping (111) and (100) surfaces of copper (Cu), an ineffective HB catalyst in its pure form. We predict the thermodynamics of two rate-limiting reactions, N 2 dissociative adsorption and the final hydrogenation step leading up to NH 3 release, at 400 and 900 K. Thermodynamically, the former reaction is favored at low temperatures, while the latter is favored at high temperatures. Vanadium-, chromium-, and molybdenum-doped Cu surfaces, due to intermediate M–N covalent bonding character, emerge as appealing candidate catalysts for PHQ NH 3 synthesis, as they balance the thermodynamics of the above-mentioned reaction steps at their respective optimal temperatures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Revealing Local Structures through Machine-Learning-Fused Multimodal Spectroscopy

Atomistic structures of materials offer valuable insights into their functionality. Determining these structures remains a fundamental challenge in materials science, especially for systems with defects. While both experimental and computational methods exist, each has limitations in resolving nanoscale structures. Core-level spectroscopies, such as X-ray absorption (XAS) or electron energy-loss spectroscopies (EELS), have been used to determine the local bonding environment and structure of materials. Recently, machine learning (ML) methods have been applied to extract structural and bonding information from XAS/EELS data. However, frameworks relying solely on a single data stream, defined as characterization data derived from a single element using one technique, are often insufficient because multiple local environments can yield similar spectral features, making it challenging to differentiate between competing structural hypotheses. Here, in this work, we address this challenge by integrating multimodal ab initio simulations, experimental data acquisition, and ML techniques for structure characterization. Our goal is to determine local structures and properties using EELS and XAS data from multiple elements and edges. To showcase our approach, we use various lithium nickel manganese cobalt (NMC) oxide compounds which are used for lithium ion batteries, including those with oxygen vacancies and antisite defects, as the sample material system. We successfully inferred local element content, ranging from lithium to transition metals, with quantitative agreement with experimental data. Beyond local element inference, we find that ML model based on multimodal spectroscopic data is able to determine whether local defects such as oxygen vacancy and antisites are present, a task which is impossible for single mode spectra or other experimental techniques. Furthermore, our framework is able to provide physical interpretability, bridging spectroscopy with the local atomic and electronic structures.

battery↗
DOE OSTI2024

Mechanistic understanding of speciated oxide growth in high entropy alloys

Abstract Complex multi-element alloys are gaining prominence for structural applications, supplementing steels, and superalloys. Understanding the impact of each element on alloy surfaces due to oxidation is vital in maintaining material integrity. This study investigates oxidation mechanisms in these alloys using a model five-element equiatomic CoCrFeNiMn alloy, in a controlled oxygen environment. The oxidation-induced surface changes correlate with each element’s interactive tendencies with the environment, guided by thermodynamics. Initial oxidation stages follow atomic size and redox potential, with the latter becoming dominant over time, causing composition inversion. The study employs in-situ atom probe tomography, transmission electron microscopy, and X-ray absorption near-edge structure techniques to elucidate the oxidation process and surface oxide structure evolution. Our findings deconvolute the mechanism for compositional and structural changes in the oxide film and will pave the way for a predictive design of complex alloys with improved resistance to oxidation under extreme conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Photoinduced evolution of lattice orthorhombicity and conceivably enhanced ferromagnetism in LaMnO 3 membranes

Ultrashort laser pulses have been utilized to dynamically drive phase transitions in correlated quantum materials. Of particular interest is whether phases not achievable in thermal equilibrium can be induced in complex oxides with intricately coupled lattice, electron and spin degrees of freedom. Here, we tracked atomic motions in LaMnO 3 following photoexcitation with MeV ultrafast electron diffraction (MeV-UED) technique. We found that the light excited state exhibits numerous signatures different from thermal equilibrium ones, including nearly conserved Bragg intensities, strongly suppressed La cation and oxygen anion displacements, and the long-range lattice orthorhombicity evolution. Furthermore, using first-principles calculations, we predict that the ferromagnetic ordering and conductivity are both enhanced upon laser excitation due to the reduction of the lattice orthorhombicity. This work benefits from recent advance in fabrication of membrane films with high epitaxial quality and in MeV-UED with large momentum space access and high temporal resolution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Simulated sulfur K-edge X-ray absorption spectroscopy database of lithium thiophosphate solid electrolytes

X-ray absorption spectroscopy (XAS) is a premier technique for materials characterization, providing key information about the local chemical environment of the absorber atom. In this work, we develop a database of sulfur K-edge XAS spectra of crystalline and amorphous lithium thiophosphate materials based on the atomic structures reported in Chem. Mater., 34, 6702 (2022). The XAS database is based on simulations using the excited electron and core-hole pseudopotential approach implemented in the Vienna Ab initio Simulation Package. Our database contains 2681 S K-edge XAS spectra for 66 crystalline and glassy structure models, making it the largest collection of first-principles computational XAS spectra for glass/ceramic lithium thiophosphates to date. This database can be used to correlate S spectral features with distinct S species based on their local coordination and short-range ordering in sulfide-based solid electrolytes. The data is openly distributed via the Materials Cloud, allowing researchers to access it for free and use it for further analysis, such as spectral fingerprinting, matching with experiments, and developing machine learning models.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ab initio calculation of X-ray and related core-level spectroscopies: Green's function approaches

X-Ray and related spectroscopies are powerful probes of atomic, vibrational, and electronic structure. In order to unlock the full potential of such experimental techniques, accurate and efficient theoretical and computational approaches are essential. Here we review the status of a variety of first-principles and nearly first principles techniques for X-ray spectroscopies such as X-ray absorption, X-ray emission, and X-ray photoemission, with a focus on Green's function based methods. In particular, we describe the current state of multiple scattering Green's function techniques available in the FEFF10 code and cumulant Green's function techniques for including the effects of many-body electronic excitations. Furthermore, illustrative examples are shown for a variety of materials and compared with other theoretical and experimental results.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗