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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 991 records · Page 55
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Freeze It or Leave It? Evaluating the Role of Cryo-Electron Microscopy in Battery Research

Cryogenic electron microscopy (cryo-EM) continues to gain prominence in materials science, particularly in battery research where it has enabled high-resolution, multimodal characterization of electrode materials and interfaces that otherwise degrade quickly under electron beam irradiation. But as anyone who has attempted cryo-EM techniques knows, freezing comes at a cost; cryo-EM experiments are time-consuming, highly sensitive, and carry an increased risk of artifacts due to issues such as frost contamination. Thus, when planning new characterization of battery materials or other beam-sensitive samples, it is critical to consider whether (and which) cryo-EM techniques are appropriate, based on study goals and an understanding of electron beam-sample interactions. Here we review such considerations for battery materials to elucidate the questions of when, why, and how to freeze to achieve high-quality characterization.

25 ENERGY STORAGE↗
DOE OSTI2025

Strain release through hydrogen bond–mediated layer twisting

Strain engineering, enabling the precise control over structure and functional properties, is a key strategy for the design of advanced materials. However, the mechanisms governing strain evolution and release at the nanoscale remain largely unexplored. In this study, we leverage in situ heating transmission electron microscopy and synchrotron x-ray spectroscopy to investigate the strain relaxation pathways of boehmite (γ-AlOOH) at 575 kelvin by revealing real-time structural dynamics. Through tracking the moiré pattern evolution, we identify distinct strain release mechanisms, including layer twisting, defect formation, and domain restructuring. Our neural network potential calculations reveal that energy fluctuations at small twist angles are dominated by an interference-like interaction modulation of hydrogen bonds between boehmite interlayers, with metastable twisted structures corresponding to local minima of the potential energy landscape. This work establishes a previously unidentified paradigm of two-dimensional layer twisting mediated by hydrogen bonding, offering insights into strain-driven transformation mechanisms, and thus may have broad implications for strain in material and earth sciences.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Small bimetallic clusters Agn-1M (M = Au, Co, Cu, Ni, Pd, Pt; n = 3, 9, 15): Density functional theory and genetic algorithm

We investigated the effect of size and composition on the properties of bimetallic nanoclusters. The geometric structures, stabilities, and electronic properties of size-selected Ag n-1 M (M = Au, Co, Cu, Ni, Pd, Pt; n = 3, 9, 15) bimetallic nanoclusters are systematically analyzed using spin-polarized density functional theory (DFT) within the generalized gradient approximation (GGA). We determine the most stable geometries for these clusters using a genetic algorithm (GA) in combination with DFT. Our results show that doping pure silver clusters with an M atom (transition metal), referred to as a “guest atom”, increases the stability as compared to pure Ag n (n = 3, 9, 15) clusters. The results for various properties including formation energy per atom, electronic structure, magnetic moments, and vibrational density of states (VDOS) are evaluated as a function of both size and composition of the system. The adsorption of selected bimetallic clusters on hydroxylated alumina substrate shows weak binding and minor changes in geometric properties except for Ag 8 Pt.

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

Deciphering the Solvation Structure of Aqueous ZnCl 2 Solutions from X-ray Absorption Spectra Using the Interpretable Graph Neural Network

Machine learning (ML) provides powerful pathways for predicting spectroscopic observables from atomic structures, but its broader impact depends on making model predictions interpretable in terms of physical and chemical principles. Here, we introduce a physics-guided graph neural network (GNN) model that predicts Zn K-edge X-ray spectroscopy (XAS) spectra of aqueous ZnCl 2 solutions. Training data are generated from ab initio XAS calculations on molecular dynamics snapshots obtained using a machine learning interatomic potential. The GNN reproduces experimental spectra across concentrations from dilute (<0.1 m) to highly concentrated (30 m, “water-in-salt”) regimes and scales efficiently to large, disordered liquid systems beyond the reach of conventional ab initio approaches. Gradient-based attribution analysis reveals that the model learns physically meaningful structure-spectrum relationships. Ligand-specific attributions reflect orbital hybridization patterns and the origin of the excitations derived from the density functional theory. Bond-length attributions recover spectral shifts consistent with multiple-scattering theory. Finally, this work bridges data-driven prediction with electronic-structure theory, establishing a general paradigm for interpretable ML that links atomic structure, electronic structure, and spectroscopic observables.

25 ENERGY STORAGE↗
DOE OSTI2025

Electrochemical Corrosion and Catalysis Dynamics of Tin Oxide during Water Oxidation

Metal oxide corrosion severely limits anodic electrocatalysis, particularly at high potentials in acidic environments, where degradation pathways remain poorly defined. This study establishes explicit connections between corrosion and electrocatalysis on tin oxide during water oxidation by examining the roles of lattice defects, reactive oxygen species, interfacial pH variations, and speciation of corroded tin in acid. We first demonstrate the presence of structural defects such as oxygen vacancies and substoichiometric Sn(II) species by integrating electron paramagnetic resonance spectroscopy, ultraviolet photoelectron spectroscopy, and Mott–Schottky analysis. Kohn–Sham density functional theory calculations reveal that explicit water structures thermodynamically stabilize reaction intermediates and lower reaction overpotentials. Moreover, we propose that water dissociation leads to hydrogen-bonding networks formed by H* and OH* intermediates, which may span the entire catalyst surface and decrease the interfacial pH to drive corrosion. In contrast, the electrochemical generation of reactive oxygen species is shown to play a minor role in catalyst corrosion during water oxidation using inductively coupled plasma mass spectrometry coupled with selective chemical scavengers. Square-wave voltammetry combined with rotating ring-disk electrodes is used to reveal that under open-circuit conditions, only Sn(IV) cations chemically dissolve from tin oxide, while both Sn(IV) and Sn(II) species electrochemically corrode during water oxidation. Our results unveil a dynamic and complicated interplay between corrosive and catalytic pathways on metal oxide electrocatalysts: a decrease in interfacial pH due to water oxidation exacerbates Sn(II)/Sn(IV) corrosion. Subsequently, the electrochemical corrosion of Sn(II)/Sn(IV) facilitates product formation from lattice oxygen, while the redeposition of corroded Sn(II) as Sn(IV) can enable oxygen exchange with water. By elucidating the roles of defects and interfacial chemistry, this work provides a roadmap for engineering improved electrocatalysts that balance activity and stability, a critical step toward scalable and durable energy technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2023

A multi-length-scale investigation of the applicability of ductility laws for annealed and work-hardened copper

Small-scale mechanical testing provides unique advantages over conventional testing in investigating the mechanical response of nuclear materials. While small-scale testing enables accelerated materials research, it raises the question of comparability to large-scale properties for engineering design considerations. Among different mechanical properties for structural design considerations such as yield and ultimate tensile stress, ductility is of critical importance with respect to structural component health. The effectiveness of using small-scale mechanical testing for probing these mechanical properties is dictated by understanding how the mechanical responses translate from the microscale to the engineering scale. Therefore, a better understanding of size scaling effects via gathering and analysis of experimental data is required to bridge length-scales. Further, this work builds upon previous reports to provide statistical data on how mechanical response changes as the size of the specimens are reduced from conventional sizes. One hundred twenty mesoscale tensile coupons of oxygen-free high thermal conductivity (OFHC) copper in work-hardened and annealed state have been manufactured using micro-wire electrical discharge machining (EDM) and tested under uniaxial tension. The mesoscale specimens have dimensions dictated by pre-selected geometric ratios (i.e., gauge section length over the square root of the cross-section area) with gauge length dimensions of 3 mm (or less) and sub-millimeter gauge widths and thicknesses. The mesoscale responses were compared to bulkscale properties to reveal the effect of specimen size on the mechanical response as a function of grain size and material state for a single phase face-centered cubic metal.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Equation of state of boron carbide B 4 ⁢C

We present the results of recent experiments conducted on the Sandia Z machine and a new tabular equation of state for B 4 ⁢C. The equation of state was calibrated to a combination of density functional calculations reported here and fits to preexisting data. It was constructed partly to recover the effects of a shock-driven, polymorphic phase transition of unknown character beginning at particle velocities of just under 3 km/s (shock pressures of 95 GPa). Some of the Z experiments included sound speeds determined by the overtaking rarefaction method, from which we calculate the Grüneisen parameter and compare with previous experiments conducted at the OMEGA laser [Fratanduono et al ., Phys. Rev. B 94 , 184107 (2016)], our own first principles calculations, and another recent tabular equation of state [Zhang et al ., Phys. Rev. E 102 , 053203 (2020)]. We also compare our results with previous static compression, thermophysical, and melt studies, finding mixed consistency. We predict the onset and completion of shock melting at 225 and 265 GPa, respectively, and predict a melt curve that is largely flat to pressures of several hundred GPa.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Shock Hugoniot calculations using on-the-fly machine learned force fields with ab initio accuracy

We present a framework for computing the shock Hugoniot using on-the-fly machine learned force field (MLFF) molecular dynamics simulations. In particular, we employ an MLFF model based on the kernel method and Bayesian linear regression to compute the free energy, atomic forces, and pressure, in conjunction with a linear regression model between the internal and free energies to compute the internal energy, with all training data generated from Kohn–Sham density functional theory (DFT). We verify the accuracy of the formalism by comparing the Hugoniot for carbon with recent Kohn–Sham DFT results in the literature. In so doing, we demonstrate that Kohn–Sham calculations for the Hugoniot can be accelerated by up to two orders of magnitude, while retaining ab initio accuracy. We apply this framework to calculate the Hugoniots of 14 materials in the FPEOS database, comprising 9 single elements and 5 compounds, between temperatures of 10 kK and 2 MK. We find good agreement with first principles results in the literature while providing tighter error bars. In addition, we confirm that the inter-element interaction in compounds decreases with temperature.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

A Porous Crystalline Nitrone-Linked Covalent Organic Framework

Herein, we report the synthesis of a nitrone-linked covalent organic framework, COF-115, by combining N, N', N', N'''-(ethene-1, 1, 2, 2-tetrayltetrakis(benzene-4, 1-diyl))tetrakis(hydroxylamine) and terephthaladehyde via a polycondensation reaction. In this study, the formation of the nitrone functionality was confirmed by solid-state 13 C multi cross-polarization magic angle spinning NMR spectroscopy of the 13 C-isotope-labeled COF-115 and Fourier-transform infrared spectroscopy. The permanent porosity of COF-115 was evaluated through low-pressure N 2 , CO 2 , and H 2 sorption experiments. Water vapor and carbon dioxide sorption analysis of COF-115 and the isoreticular imine-linked COF indicated a superior potential of N-oxide-based porous materials for atmospheric water harvesting and CO 2 capture applications. Density functional theory calculations provided valuable insights into the difference between the adsorption properties of these COFs. Lastly, photoinduced rearrangement of COF-115 to the associated amide-linked material was successfully demonstrated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Colloidal CdSe nanocrystals are inherently defective

Abstract Colloidal CdSe nanocrystals (NCs) have shown promise in applications ranging from LED displays to medical imaging. Their unique photophysics depend sensitively on the presence or absence of surface defects. Using simulations, we show that CdSe NCs are inherently defective; even for stoichiometric NCs with perfect ligand passivation and no vacancies or defects, we still observe that the low energy spectrum is dominated by dark, surface-associated excitations, which are more numerous in larger NCs. Surface structure analysis shows that the majority of these states involve holes that are localized on two-coordinate Se atoms. As chalcogenide atoms are not passivated by any Lewis base ligand, varying the ligand should not dramatically change the number of dark states, which we confirm by simulating three passivation schemes. Our results have significant implications for understanding CdSe NC photophysics, and suggest that photochemistry and short-range photoinduced charge transfer should be much more facile than previously anticipated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Pump and ionizing-probe dynamics in a simultaneous treatment of electronic and nuclear motion in LiH

The dissociative single ionization of the LiH molecule using a two-color UV-UV pump-probe scheme is simulated in ab initio calculations demonstrating how the dynamics initiated on intermediate Rydberg states of diatomic molecules can be imaged by such experiments. The theoretical treatment combines nuclear motion with highly correlated descriptions of electronic continua and bound electronic states. Nuclear dynamics on Rydberg states are only weakly reflected by changes in photoelectron energies ejected by time-delayed ionizing pulses if the Rydberg potential curves parallel those of the ion states being produced. However, coincidence measurements guided by knowledge of the photoionization amplitudes as a function of internuclear distance can still reveal intermediate-state dynamics in pump-probe experiments.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Quantum Computation of Dynamical Quantum Phase Transitions and Entanglement Tomography in a Lattice Gauge Theory

Strongly coupled gauge theories far from equilibrium may exhibit unique features that could illuminate the physics of the early universe and of hadron and ion colliders. Studying real-time phenomena has proven challenging with classical-simulation methods but is a natural application of quantum simulation. To demonstrate this prospect, we quantum compute nonequal-time correlation functions and perform entanglement tomography of nonequilibrium states of a simple lattice gauge theory, the Schwinger model, using a trapped-ion quantum computer by IonQ Inc. As an ideal target for near-term devices, a recently predicted dynamical quantum phase transition in this model is studied by preparing, quenching, and tracking the subsequent nonequilibrium dynamics in three ways: (i) overlap echos signaling dynamical transitions, (ii) nonequal-time correlation functions with an underlying topological nature, and (iii) the entanglement structure of nonequilibrium states, including entanglement Hamiltonians. These results constitute the first observation of a dynamical quantum phase transition in a lattice gauge theory on a quantum computer and are a first step toward investigating topological phenomena in nuclear and high-energy physics using quantum technologies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Intertwined charge and spin density waves in a topological kagome material

Using neutrons and x rays we show the topological kagome antiferromagnet Mn 3 Sn for T < 285 K forms a homogeneous spin and charge ordered state comprising a longitudinally polarized spin density wave with wave vector k β = k β c ̂ , a helical modulated version of the room temperature antichiral magnetic order with k χ = k χ c ̂ , and charge density waves with wave vectors 2 k β , 2 k χ , and k β + k χ . Though k χ and k β coincide for 200 K < T < 230 K , they exhibit distinct continuous T dependencies before locking to commensurate values of k β = 1 12 c * and k χ = 5 48 c * at low T . Density functional theory indicates this complex modulated state may be associated with the nesting of Fermi surfaces from correlated flat kagome bands, which host Weyl nodes that are annihilated as it forms. Published by the American Physical Society 2024

Chen, Y. (ORCID:0000000177169179)↗
DOE OSTI2025

Defect formation and microstructure tuning via proton irradiation to control electrochemical and phase reversibility in layered battery materials

The reversibility of phase transformation influences the functionality of electrode materials in batteries. In many battery materials, nanosized grains favor phase reversibility but at the cost of cyclability due to aggravated side reactions with the electrolyte. Here, in this study, we present a novel approach to enhance the phase transformation reversibility of layered oxide cathodes, exemplified by Na 2/3 Fe 1/2 Mn 1/2 O 2 through proton irradiation. In addition to forming defects, proton irradiation at sufficiently high doses can subdivide single grains into multiple nanodomains without physically rupturing them. Hence, the single grains of the material assume a pseudo-secondary particle nature without reducing the overall grain size. Preserving the grain size is advantageous, as it reduces side reactions, which is not possible with conventional grain size reduction methods. While chemical transformations and defect formation induced through proton irradiation can influence the stability of battery materials, it is expected that structural reorganization due to cycling-induced phase transformation will be contained within these nanodomains. Such confinement of phase transformation is potentially responsible for enhancing the reversibility of layered oxide materials in our study. Thus, our study suggests that grain subdivision could become an effective microstructure tuning strategy for managing electrochemical cycling-induced phase changes in battery electrodes.

25 ENERGY STORAGE↗
DOE OSTI2022

Cesium-mediated electron redistribution and electron-electron interaction in high-pressure metallic CsPbI3

Abstract Electron-phonon coupling was believed to govern the carrier transport in halide perovskites and related phases. Here we demonstrate that electron-electron interaction enhanced by Cs-involved electron redistribution plays a direct and prominent role in the low-temperature electrical transport of compressed CsPbI 3 and renders Fermi liquid (FL)-like behavior. By compressing δ-CsPbI 3 to 80 GPa, an insulator-semimetal-metal transition occurs, concomitant with the completion of a slow structural transition from the one-dimensional Pnma (δ) phase to a three-dimensional Pmn 2 1 (ε) phase. Deviation from FL behavior is observed upon CsPbI 3 entering the metallic ε phase, which progressively evolves into a FL-like state at 186 GPa. First-principles density functional theory calculations reveal that the enhanced electron-electron coupling results from the sudden increase of the 5d state occupation in Cs and I atoms. Our study presents a promising strategy of cationic manipulation for tuning the electronic structure and carrier scattering of halide perovskites at high pressure.

36 MATERIALS SCIENCE↗
DOE OSTI2024

High-Pressure Rate Rules for Ether Alkylperoxy Radical Isomerization

The first isomerization reaction of an alkylperoxy (RO 2 ) radical holds significant importance in low-temperature oxidation, as it governs the branching ratios of the hydroperoxyalkyl (QOOH) radicals, which influence the competition between the chain-propagation and chain-branching reactions. In this study, we systematically calculated high-pressure rate rules for the RO 2 isomerization reaction of monoethers, exploring 5-, 6-, 7-, and 8-membered ring transition states. Primary, secondary, and tertiary carbon sites, where both the abstracting peroxy group and the abstracted hydrogen are located, were considered, with particular emphasis on distinguishing between secondary carbons adjacent (alpha) and nonadjacent to the ether functional group. Using the G4//B3LYP/6-311++G(2df,2pd) level of theory and the transition state theory, we estimated the rate constants and the Arrhenius coefficient for over 120 possible isomerization reactions. We examined the effect of ring size and ring atoms, revealing that 6- and 7-membered ring isomerizations were generally the fastest. The impact of the ether functional group on transition states was investigated by comparing reactions with identical ring size, peroxy, and radical positions, but with the ether functional group positioned either outside (i.e., out) or inside (i.e., in) the transition state ring, leading to differences in the rate constants. When comparing to analogous alkane rate constants, differences of up to an order of magnitude were observed, underscoring the need for caution when assigning rate rules by analogy. We applied our rate constants in the di-iso-butyl ether kinetic model and evaluated their influence on low-temperature chemistry finding that they altered the branching ratios by up to a factor of 9, highlighting the significance of site-specific rate constants for more accurate low-temperature modeling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Electric Field Control of Magnetic Skyrmion Helicity in a Centrosymmetric 2D van der Waals Magnet

Two-dimensional van der Waals magnets hosting topological magnetic textures, such as skyrmions, show promise for spintronics and quantum computing. Electrical control of these topological spin textures is crucial for enhancing operational performance and functionality. Here, using electron microscopy combined with in situ electric and magnetic biasing, we show that the skyrmion helicity in insulating Cr 2 Ge 2 Te 6 can be controlled by the direction of the external electric field applied during the field cooling process. The electric field-tuned helicity remains stable at low temperature, even amid variations in magnetic and electric fields. Our theoretical investigation reveals that nonzero Dzyaloshinskii-Moriya interactions between nearest neighbors, induced by the electric field, change their sign upon reversing the electric field direction, thereby facilitating helicity selection. The electrical control of magnetic helicity demonstrated in this study can be extended to other centrosymmetric skyrmion-hosting magnets, paving the way for future device designs in topological spintronics and quantum computing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Nonradiative relaxation dynamics in the [Au 25- n Ag n (SH) 18 ] -1 ( n = 1, 12, 25) thiolate-protected nanoclusters

Evaluation of the electron-nuclear dynamics and relaxation mechanisms of gold and silver nanoclusters and their alloys is important for future photocatalytic, light harvesting, and photoluminescence applications of these systems. In this work, the effect of silver doping on the nonradiative excited state relaxation dynamics of the atomically precise thiolate-protected gold nanocluster [Au 25- n Ag n (SH) 18 ] –1 ( n = 1, 12, 25) is studied theoretically. Time-dependent density functional theory is used to study excited states lying in the energy range 0.0–2.5 eV. The fewest switches surface hopping method with decoherence correction was used to investigate the dynamics of these states. The HOMO–LUMO gap increases significantly upon doping of 12 silver atoms but decreases for the pure silver nanocluster. Doped clusters show a different response for ground state population increase lifetimes and excited state population decay times in comparison to the undoped system. The ground state recovery times of the S 1 –S 6 states in the first excited peak were found to be longer for [Au 13 Ag 12 (SH) 18 ] –1 than the corresponding recovery times of other studied nanoclusters, suggesting that this partially doped nanocluster is best for preserving electrons in an excited state. The decay time constants were in the range of 2.0–20 ps for the six lowest energy excited states. Among the higher excited states, S 7 has the slowest decay time constant although it occurs more quickly than S 1 decay. Overall, these clusters follow common decay time constant trends and relaxation mechanisms due to the similarities in their electronic structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗