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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Determining the Ensemble N -Representability of Reduced Density Matrices

The N-representability problem for reduced density matrices remains a fundamental challenge in electronic structure theory. Following our previous work that employs a unitary-evolution algorithm based on an adaptive derivative-assembled pseudo-Trotter variational quantum algorithm to probe pure-state N-representability of reduced density matrices [J. Chem. Theory Comput. 2024, 20, 9968], in this work we propose a practical framework for determining the ensemble N-representability of a p-body matrix. This is accomplished using a purification strategy that embeds an ensemble state into a pure state defined on an extended Hilbert space, such that the reduced density matrices of the purified state reproduce those of the original ensemble. By iteratively applying variational unitaries to an initial purified state, the proposed algorithm minimizes the Hilbert-Schmidt distance between its p-body reduced density matrix and a specified target p-body matrix, which serves as a measure of the N-representability of the target. This methodology facilitates both error correction of defective ensemble reduced density matrices and quantum-state reconstruction on a quantum computer, offering a route for density-matrix refinement. We validate the algorithm with numerical simulations on systems of two, three, and four electrons in both simple models as well as molecular systems at finite temperature, demonstrating its robustness.

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

Investigation of magnetic fluctuations in L-H and H-L transition dynamics on DIII-D

The dynamics of the L-H transition is not fully understood, with many parameters changing the threshold power to enter H-mode and the self-regulation between zonal flows and turbulence in the plasma edge. This paper is primarily a presentation of experimental results for DIII-D L-H and H-L transitions and speculation on the observations made. Power threshold analysis and measurements of pedestal temperatures for these transitions are presented. A comparison is made between an L-H transition and H-L transition of comparable Psep exhibiting oscillatory behaviour, showing symmetry between forward and backward transition dynamics. This paper shows the first observations of magnetic fluctuations during L-H and H-L transitions on DIII-D, and shows that L-H and H-L transitions have similar magnetic fluctuation dynamics. Information geometry analysis has been performed on measurements of plasma density fluctuations, perpendicular plasma velocity fluctuations, and magnetic field fluctuations to investigate the self-regulation and evolution of these variables during the transitions. Perpendicular flow evolution is shown to dominate the transition dynamics in both directions, but self-regulation behaviour is observed between all three variables. A strong correlation between magnetic fluctuation information rate and density fluctuation information rate for these two shots shows the strong influence of magnetic behaviour on both the L-H and H-L transition, and that these transition dynamics necessarily include electromagnetic effects.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2026

Combining ToF‐SIMS and Multivariate Analysis to Resolve Active Sites on Ni‐Based HER Catalysts

Unambiguous identification of active sites in heterogeneous catalysis remains a major challenge, particularly for materials with ultrathin, chemically mixed surface layers. Here, we demonstrate a generalizable approach that combines time-of-flight secondary ion mass spectrometry (ToF-SIMS) with multivariate statistical analysis (principal component analysis [PCA] and multivariate curve resolution [MCR]) to resolve catalytically relevant motifs at the nanoscale. Using Ni electrodes as a model system, PCA distinguished hydroxide-enriched domains from oxide- and metal-rich regions, while MCR decomposed depth profiles and 3D images into hydroxide, oxide, and metallic layers with nanometer resolution. A unique secondary-ion fragment, NiO 3 H 3 − (m/z 108.94), emerged as a marker of hydroxide-rich environments and correlated with hydrogen evolution reaction (HER) activity across a series of Ni electrodes. Complementary density functional theory (DFT) calculations revealed that Ni(OH) 2 clusters adjacent to metallic Ni offer the most favorable water dissociation energetics, establishing the structural origin of the marker. While illustrated here for Ni-based HER, this workflow provides a broadly applicable framework to isolate and rank near-surface patterns that govern catalytic activity, thereby extending ToF-SIMS from a qualitative probe to a predictive tool for active site identification.

HER active sites↗
DOE OSTI2025

Modulation of thermal conductivity of iron-doped ß-Ga2O3 by helium-ion irradiation

This study examines the impact of helium-ion irradiation on the thermal conductivity of ß-Ga2O3. A laser-based spatial domain thermoreflectance technique is used to investigate thermal conductivity map for both un-irradiated and irradiated ß-Ga2O3, which are then validated against simulation results derived from density functional theory-based phonon transport simulations. Since helium bubble evolution was ob- served at the nanoscale using transmission electron microscopy, the simulation study was carried out on eight distinct helium-induced sites in ß-Ga2O3. Our findings indicate a reduction in thermal conductivity for the irradiated samples. Experimental results show a significant reduction in thermal conductivity in irradiated samples, with de- creases of approximately 25% along the [100] direction and 40% along [001] directions. Phonon transport simulations closely replicate these findings, particularly when helium occupying interstitial sites, predicting reductions of ˜53% along [100] and ˜50% along [001] directions. This work underscores the role of irradiation-induced microstructural changes in the heat transport properties of ß-Ga2O3 which is crucial for its application in sensor devices in extreme environments.

36 - MATERIALS SCIENCE↗
DOE OSTI2025

A phase-field fracture formulation for generalized standard materials: The interplay between thermomechanics and damage

Accurately modeling fracture of ductile materials poses open challenges in the field of computational mechanics due to the multiphysics nature of their failure processes. Integrating the interplay between thermodynamics and damage into ductile fracture models is vital for predicting critical failure modes. Here, in this paper, we develop a versatile phase-field (PF) framework for modeling ductile fracture, taking into account finite-strain elasto-plasticity. The framework stems from a variational formulation of constitutive relations for generalized standard materials (GSMs), whose response is described by a Helmholtz free energy and a dissipation pseudo-potential. Its variational structure is based on a minimum principle for a functional that expresses the sum of power densities for reversible and irreversible processes. By minimizing this functional with a constraint on a von Mises yield function, we derive the evolution equation for the equivalent plastic strain and an associative flow rule. This constrained optimization problem is analytically solved for a wide class of thermo-viscoplasticity models. The key innovations of the current work include (i) a cubic plastic degradation function that accounts for a non-vanishing damage-dependent yield stress, (ii) closed-form expressions of the Helmholtz free energy and dissipation pseudo-potential for three thermo-viscoplasticity models, (iii) an extended Johnson–Cook plasticity model with a nonlinear hardening law, and (iv) a plastic work heat source that depends on the plastic degradation function and a variable Taylor–Quinney (TQ) coefficient. The capabilities of the proposed framework are tested with the aid of four ductile fracture problems, including the Sandia Fracture Challenge. In each of these problems, we examine the evolution of relevant field variables such as the PF order parameter, the equivalent plastic strain, the temperature, and the internal power dissipation density, in addition to the overall structural response quantified by the force–displacement curve. These numerical studies demonstrate that the proposed framework effectively represents ductile fracture, yielding computational results that exhibit good agreement with experimental data.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Interplay of Quantum Size Effect and Tensile Strain on Surface Morphology of β-Sn(100) Islands

The quantum size effect (QSE) and strain effect are two key factors influencing the surface morphology of thin films, which can increase film surface roughness through QSE-induced thickness oscillation and strain-induced island formation, respectively. Surface roughness usually manifests in the early stages of film growth and diminishes beyond a critical thickness. In this work, we employ molecular beam epitaxy (MBE) to grow β-Sn(100) islands with varying thickness N on bilayer graphene-terminated 6H-SiC(0001) substrates. Scanning tunneling microscopy and spectroscopy measurements reveal an inverse surface roughness effect that highlights the interplay of QSE and misfit strain in shaping the surface morphology of β-Sn(100) islands. For N ≤ 10, the islands exhibit flat surfaces, while for N ≥ 26, the island surfaces become corrugated and patterned. For the intermediate range, i.e., 12 ≤ N ≤ 24, both flat and patterned surfaces coexist, with the percentage coverage of the patterned surface oscillating as a function of N. By performing density functional theory calculations, we demonstrate that the unusual surface pattern evolution in our MBE-grown β-Sn(100) islands is a result of the interplay between QSE-induced surface roughing and tensile strain-induced smoothening effect.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Operando Unveiling of Hydrogen Spillover Mechanisms on Tungsten Oxide Surfaces

Hydrogen spillover is an important process in catalytic hydrogenation reactions, facilitating H 2 activation and modulating surface chemistry of reducible oxide catalysts. This study focuses on the operando unveiling of platinum-induced hydrogen spillover on monoclinic tungsten trioxide (γ-WO 3 ), employing ambient pressure X-ray photoelectron spectroscopy, density functional theory calculations and microkinetic modeling to investigate the dynamic evolution of surface states at varied temperatures. At room temperature, hydrogen spillover results in the formation of W 5+ and hydrogen intermediates (hydroxyl species and adsorbed water), facilitated by Pt metal clusters. With increasing temperature, water desorption, reverse hydrogen spillover and surface-to-bulk diffusion of hydrogen atoms compete with each other, leading initially to reoxidation and then further reduction of W atoms in the near-surface. The combined experimental results and simulations provide a comprehensive understanding of the mechanisms underlying hydrogen interaction with reducible metal oxides, lending insights of relevance to the design of enhanced hydrogenation catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Dynamical friction in dark matter superfluids: The evolution of black hole binaries

Abstract The theory of superfluid dark matter is characterized by self-interacting sub-eV particles that thermalize and condense to form a superfluid core in galaxies. Massive black holes at the center of galaxies, however, modify the dark matter distribution and result in a density enhancement in their vicinity known as dark matter spikes. The presence of these spikes affects the evolution of binary systems by modifying their gravitational wave emission and inducing dynamical friction effects on the orbiting bodies. In this work, we assess the role of dynamical friction for bodies moving through a superfluid core enhanced by a central massive black hole. As a first step, we compute the dynamical friction force experienced by bodies moving in a circular orbit. Then, we estimate the gravitational wave dephasing of the binary, showing that the effect of the superfluid drag force is beyond the reach of space-based experiments like LISA, contrarily to collisionless dark matter, therefore providing an opportunity to distinguish these dark matter models.

Astronomy & Astrophysics↗
DOE OSTI2025

Off-Equilibrium Reactivity of Boron-Enriched Metal Diboride Surfaces in Electroreduction Conditions

Boron-based materials, featuring B-dependent reactivity and diverse phases, are emerging as promising catalyst systems. However, the catalytic mechanism on many borides remains poorly understood due to complex surface reconstructions under reaction conditions. Here, we investigate the MoB 2 surface in conditions of hydrogen evolution reaction in acidic media, using grand canonical global optimization, grand canonical density functional theory, ab initio molecular dynamics, free energy surface sampling, and an analytical model for electrochemical barrier evaluation. We propose a boron-enrichment strategy to tune the surface reactivity of the hexagonal face of MoB 2 . We reveal the dynamic nature of the B-enriched surface under H coverage and kinetic trapping of the system in the metastable regime with an extensive examination of the deactivation pathways. The metastable center B site on B-enriched surfaces, featuring buckled-up configuration and a usual relaxation effect, is found to be highly active toward HER via the Volmer–Heyrovsky mechanism. In conclusion, this work demonstrates how off-equilibrium behaviors can arise from the interplay between adsorbate coverage and surface reconstruction on a seemingly simple surface, and we present a theoretical framework and computational workflows to address these behaviors, along with other realistic complexities, in kinetics simulations.

Adsorption↗
DOE OSTI2025

Establishing defect-property relationships for 2D-nanomaterials (Final technical report)

Studies of new families of two-dimensional nanomaterials (2DNMs) have established that they possess unique properties that diverge from those of their bulk counterparts. This project aimed to determine how tolerant 2DNMs are to extreme photon and particle fluxes and to identify the mechanisms governing their radiation response. Early work indicated that graphene is not as representative of other 2DNMs as previously assumed; however, the origin of this difference remained unclear. To address these knowledge gaps, this project investigated the physical processes occurring at multiple length scales in transition metal dichalcogenides (TMDs) and quantified their structural stability and property evolution under far-from-equilibrium conditions. In-situ and ex-situ ion and electron irradiations were performed to directly control and monitor defect formation in TMDs. Complementary density functional theory (DFT) and molecular dynamics (MD) simulations were employed to elucidate the mechanisms of defect generation and evolution. The outcomes of this work established mechanistic understanding of irradiation-induced defect formation in 2DNMs, quantified the radiation tolerance of TMDs, and built a fundamental knowledge base for correlating defect structures with material properties. Collectively, these results provide new insights into the stability of low-dimensional materials in extreme environments and enable the predictive design of radiation-tolerant 2DNMs.

2D materials↗
DOE OSTI2025

Experimental study of high-energy single-pulse nanosecond discharges in pin-to-pin configuration

Single-pulse pin-to-pin nanosecond pulsed discharges in ambient air (gap distances of 3–7 mm) were investigated at high pulse energies (∼20–30 mJ deposited energy per 11 ns full width at half maximum pulse). A Michelson interferometry setup (532 nm continuous-wave laser) was employed to record time-resolved interferograms of the discharge, enabling spatially resolved calculation of the electron number density. An intensified charge-coupled device camera was used to capture the spatiotemporal evolution of the discharge (streamer formation and spark channel development), and Coherent Anti-Stokes Raman Spectroscopy (CARS) was used to measure post-discharge N 2 vibrational temperatures. Discharge current and voltage were monitored with a back-current shunt. The discharge was initiated with simultaneous cathode-directed and anode-directed streamers that bridge the gap within ∼1 ns and form a luminous, filamentary plasma channel immediately after breakdown. Laser interferometry measurements showed peak electron number densities of the order of 10 1 7–10 18 cm −3 , occurring about 15–20 ns after pulse arrival at the discharge gap. Shorter gap discharges yielded higher peak electron densities, consistent with the higher energy density in the smaller gaps. Spatially, the electron density was highest near the electrodes and decreased toward the midgap region, with 5 and 7 mm gaps exhibiting a pronounced drop in the central channel. CARS indicated initial vibrational temperatures of approximately 4000–6000 K in the spark core of ∼50 ns after the discharge onset, decaying on a ∼500 ns timescale as the plasma cooled and recombined.

Coherent anti-Stokes Raman spectroscopy↗
DOE OSTI2026

Modeling the influence of the solid electrolyte interphase on the sand’s time and dendrite formation on lithium metal electrodes

Lithium metal is a sought after battery material for its high energy density due to the low electrochemical potential and density. However, lithium metal is also highly reactive, which results in a strong propensity for dendrite formation. The Sand’s time has previously been used to predict the time of dendrite initiation on metals that do not form a solid-electrolyte interphase (SEI), but it has been shown that the Sand’s time is not accurate for lithium electrodes when using transport parameters associated with the electrolyte. Thus, we built a numerical model to simulate lithium ion transport through a growing SEI to predict the Sand’s time. The numerical model is shown to be more accurate than previous analytical solutions, especially for low current densities. We then analyze the sensitivity of the Sand’s time to different SEI properties and the chemical potential gradients present in the SEI, driving lithium transport. The results showed that high lithium concentration has a greater impact at high current density, while fast diffusivity is more important at low current density. Lastly, we modeled the influence of surface roughness on the plating evolution and chemical potential gradients when an SEI is present in comparison to the electrolyte. As a result, we demonstrate that the SEI plays a critical role in lithium electrode stability, and that improved characterization techniques are needed to better understand transport through the SEI and increase lithium metal utilization in energy storage devices.

Chemistry↗
DOE OSTI2026

A new self-adaptive reconstruction method to identify defects through Wigner–Seitz approach

A new self-adaptive reconstruction method based on local atomic structure at any given molecular dynamics (MD) step has been developed in this article. The method can be used in Wigner–Seitz defect analysis approach to correctly and efficiently explore the information of both point defects and complex defect clusters (e.g. dislocation loops and voids) formed after a displacement cascade where the cascade interacts with grain boundaries and/or dislocations. The algorithm and validation are provided in detail. Results for identification of radiation defects during and after cascades interacting with a dislocation network show that the new method can well recognize all simple and complex defects and defect clusters. Thus, this new method provides a totally new way to explore the density and size of radiation defects at atomic scale after complex MD evolution processes, providing correct information to understand and predict radiation damage in materials through atomic simulations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Synthesis of multicomponent oxygen evolution reaction coatings via block copolymer templating with vapor- and solution-phase precursors

Porous mixed transition metal oxide heterostructures are promising electrocatalysts due to their high surface area. However, achieving conformal multicomponent oxide coatings with controlled nanoscale architectures remains challenging. Here, we report a synthesis strategy that integrates solution-based swelling infiltration (SBI) with gas-phase sequential infiltration synthesis (SIS) in a block copolymer template to fabricate porous, high-surface-area, conformal mixed-oxide electrocatalytic coatings. In this approach, a PS75-P4VP25 block copolymer (BCP) film is first infiltrated with transition metal acetylacetonate precursors via SBI, followed by exposure to gas phase precursors of ZnO via SIS process. Thermal annealing of the infiltrated BCP films converts them into all-inorganic Fe–ZnO, Fe–Co–ZnO, and Fe–Ni–ZnO coatings. Electrochemical testing on 70 nm thick conformal coatings demonstrates promising oxygen evolution reaction (OER) activity in alkaline media, with mass-specific current densities up to 1.0 × 10 5 mA/g at an overpotential of 330 mV (vs. RHE) at ultralow loading (~0.005 g/cm 2 ). Among the compositions, Fe–Co–ZnO and amorphous Fe–Ni–ZnO show the best OER performance, delivering current densities of 2.00 and 3.04 mA/cm 2 , respectively, compared to 1.52 mA/cm 2 for Fe–ZnO.. This work establishes SBI–SIS as a versatile route for fabricating nm-thin, high-performance multicomponent oxide heterostructures on cost-efficient supports, enabling efficient catalyst utilization in electrochemical energy conversion application.

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

Cyclodextrin-Derived Porous Liquids Enabled by In Situ Solvation Shell Formation

Porous liquids (PLs) represent a unique platform for molecular separations by combining permanent porosity with liquid-phase mobility. However, it remains a formidable challenge to construct and stabilize PLs with sub-5 Å pores using readily available porous host and liquid media. Here, we report the construction of cyclodextrin (CD)-derived PLs enabled by in situ solvation shell formation. The acid–base neutralization reaction between CD and an organic base was leveraged to generate a thin ionic solvation shell around the CD host, effectively liquefying CD and preventing its segregation in the liquid base medium while preserving accessible molecular-scale cavities. Spectroscopic analysis, neutron scattering, density functional theory calculations, and molecular dynamics simulations collectively confirm the structural evolution and existence of abundant internal porosity in PLs. The unique architectures of CD-derived PLs enable highly selective encapsulation of fluorinated alkanes and significantly enhanced uptake of inert gases. This facile and generalizable strategy enables construction of high-quality PLs with engineered ultramicroporosity to facilitate molecular separations.

Cavities↗
DOE OSTI2026

Interfacial Charge Transfer Pathways in Photoelectrochemical H 2 Evolution by a Single-Component Molecular Catalyst on a Conductive Metal Oxide

Dye-sensitized photoelectrosynthesis cells traditionally combine a photosensitizing dye to harvest light and a catalyst to generate chemical fuels on a semiconductor. Here, in this work, a photoactive catalyst capable of both light absorption and fuel formation, [Cp*Ir(4,4′-Y 2 -bpy)Cl][Cl] (Cp* = pentamethylcyclopentadienyl, bpy = 2,2′-bipyridine, Y = CH 2 PO 3 H 2 ), is anchored to a mesoporous tin-doped indium oxide (ITO) electrode and facilitates photoelectrochemical H 2 evolution in water without the need for additional photosensitizers or sacrificial reductants. Spectroelectrochemistry indicates a single-site H 2 evolution mechanism involving charge injection to ITO, in contrast to the bimetallic mechanism observed in solution. Cyclic voltammetry and variable-potential chronoamperometry under illumination probe competing pathways via interfacial electron transfer between the Ir hydride excited state and the conductive ITO electrode. A Marcus theory framework provides reorganization energies for competing interfacial electron transfer pathways from potential-dependent quantum yield measurements. The light-driven H 2 evolution catalysis on conducting oxide proceeds with high Faradaic efficiency and current densities comparable to photoelectrodes utilizing p-type semiconductors. By uncovering the principal electron transfer pathways that govern photocatalytic efficiency, this study establishes design principles for hybrid molecular photoelectrocatalysts.

catalysts↗
DOE OSTI2024

Phenomenology of TMD parton distributions in Drell-Yan and 𝑍 0 boson production in a hadron structure oriented approach

We present a first practical implementation of a recently proposed hadron structure oriented (HSO) approach to transverse momentum dependent (TMD) phenomenology applied to Drell-Yan-like processes, including lepton pair production at moderate 𝑄 2 and 𝑍 0 boson production. We compare and contrast general features of our methodology with other common practices and emphasize aspects that we view as improvements. Separately, we discuss the importance of treatments that preserve various theoretical properties of the nonperturbative parts of TMD parametrizations for future applications that have the extraction of hadron structure as a primary goal. These include the HSO’s preservation of a basic TMD parton-model-like framework even while accounting for full TMD factorization and evolution, explicit preservation of the integral relationship between TMD and collinear parton density functions, and the ability to meaningfully compare different theoretical models of nonperturbative TMD parton distributions. In our examples, we show that there is significant sensitivity at moderate 𝑄 2 to both the form of the nonperturbative transverse momentum dependence and the parametrization of collinear parton densities. However, we also find that evolving to 𝑄 2 =𝑀$^2_𝑍$, without fitting, results in a satisfactory postdiction of existing data for 𝑍0 production, nearly independently of the modeling of nonperturbative transverse momentum behavior. We argue that this demonstrates that moderate 𝑄 measurements should be given greater weight than high 𝑄 measurements in extractions of nonperturbative transverse momentum dependence. We also obtain new extractions of the nonperturbative Collins-Soper kernel within the HSO approach. We discuss its features and compare with some earlier extractions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗