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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

High-throughput investigation of structural evolution upon solid-state in Cu–Cr–Co combinatorial multilayer thin-film

Cu-Cr-Co combinatorial multilayer thin-films were prepared by a high-throughput ion beam sputtering system. Based on the thickness ratio among the individual nanoscale monolayers (Cu, Cr, Co), the resulting stoichiometry covered the entire phase diagram. The chemical composition and structure of Cu-Cr-Co combinatorial chip upon solid-state reaction were studied by lab-based micro-X-ray fluorescence (mu-XRF) and high-throughput synchrotron X-ray diffraction (XRD), respectively. A composition-structure map for Cu-Cr-Co combinatorial chip was developed through automated data analysis employing hierarchical clustering techniques. The structural evolution of Cu-Cr-Co combinatorial chip as a function of heat-treatment temperature, time, and modulation period were studied systematically. Furthermore, the effect of the elemental distribution in-depth direction was investigated to gain more insights regarding phase transformation. This work provides an efficient method and new perspectives for the design and optimization of the composition and structure of high-performance thin-films.

36 MATERIALS SCIENCE↗
DOE OSTI2025

A versatile and practical synthesis of oxygen evolution catalysts

State-of-the-art OER (oxygen evolution reaction) catalyst syntheses require the use of expensive metals (i.e. Ir) with complex and time-consuming synthetic routes, difficulty in control, and impractical yields. Although some reported catalysts show improved performance (i.e. activity, stability, lowering Ir content with Ru), their synthesis is costly and not viable for scale-up. Here we demonstrate a practical, reliable, and scalable one-pot synthesis method for OER catalysts based on borohydride reduction to quickly yield >100 mg of Ir, Ru, and IrRu nanoparticles (1.6 ± 0.2 nm) with outstanding batch-to-batch consistency. Both mono- and bi-metallic compositions exhibit a metal-core/metal-oxide-shell nanoparticle structure. We further demonstrate the versatility of this method by incorporating earth-abundant yttrium, resulting in a catalyst with improved precious metal utilization for OER. This method serves as a robust platform for generating ultrasmall (<2 nm) multi-metal particles useful for electrocatalysis research.

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

Kinetics and evolution of solid-state metal dealloying in thin films with multimodal analysis

Thin-film solid-state metal dealloying (thin-film SSMD) is an emerging technique that uses self-organization to design nanostructured thin films. The resulting 3D bicontinuous nanostructures are promising for a wide range of applications, such as catalysis and energy storage. In this work, we prepared thin films by SSMD using Ti-Cu as the parent alloy and Mg as the solvent. Using a multimodal approach, we combined synchrotron X-ray spectroscopy, diffraction, and high-resolution electron-based spectroscopy and imaging to study their morphological, structural, and chemical evolution. The processing-structure relationship was analyzed as a function of parent alloy composition and dealloying temperature and time. Morphological transitions from globular, to lamellar, to bicontinuous structures, in conjunction with a ligament size evolution, were identified as functions of the parent alloy composition. The dealloying rate increased with increasing concentration of interdiffusing elements (dissolving component) in the parent alloy. The parting limit, a dealloying compositional threshold, was systematically analyzed and determined to be 30%–40%. The order of crystalline phase formation is CuMg 2 , Cu 2 Mg, and Ti; the Ti phase first shows self-reorganization during dealloying, separate from the crystallization process. The coarsening in thin-film SSMD was identified and not entirely self-similar; in addition to the increase of ligament size over time, the formation of larger globular ligaments were also observed. This work furthers our fundamental understanding of thin-film SSMD and nanostructured thin-film design, where the thermodynamic and kinetic effects differ from the bulk counterparts. The fact that dealloying and diffusion outpaces the crystallization and new phase formation also offers opportunities to utilize thin-film SSMD in certain alloy systems in which deleterious intermetallic phases need to be suppressed, that may not be possible in the bulk geometry.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Solid-state reaction mediated microstructural evolution in a spark plasma sintered in situ Ti–B 4 C composite

For this study, a novel porosity-free in situ Ti–B 4 C composite was fabricated via spark plasma sintering (SPS). Detailed analysis of the phase evolution, coupling results from XRM, XRD and SEM-EBSD-EDS, indicate that primarily TiB 2 precipitates formed due to the in-situ reactions between the boron-carbide and titanium powders. The precipitation of TiB 2 resulted in the formation of a graphitic C-rich thin layer circumscribing the partially reacted B 4 C particles. Further progression of the in-situ reaction leads to the out-diffusion of the excess carbon from the B 4 C particles, across the graphite and TiB 2 phases, forming TiC upon reacting with the titanium matrix. Therefore, the final microstructure primarily consisted of TiB 2 , TiC, and partially reacted B 4 C phases, with small amounts of TiB, α-Ti, and graphite. Furthermore, the microstructure in these SPS processed in situ composites appeared to be the product of a solid-state Ti–B 4 C diffusion couple, substantially different from their fusion-based additively manufactured counterparts. Nano-indentation tests revealed a remarkably high average hardness of ~25 GPa for this SPS-processed Ti–B 4 C composite and comparable (with literature) phase-specific hardness and modulus values for the constituent TiB 2 , TiC, and B 4 C phases.

36 MATERIALS SCIENCE↗
DOE OSTI2023

The Classical Equations of Motion of Quantized Gauge Theories, Part I: General Relativity

In this and a companion paper, we show that quantum field theories with gauge symmetries permit a broader class of classical dynamics than typically assumed. In this article, we show that the dynamics extracted from the path integral or Hamiltonian formulation of general relativity allows for classical states that do not satisfy the full set of Einstein's equations. This amounts to loosening the Hamiltonian and momentum constraints that are imposed on the initial state. Nevertheless, the quantum theory permits gauge invariant time evolution of these states. The time evolution of these states is such that at the classical level the full set of Einstein's equations would appear to hold, with the physical effects of these states being attributable to an auxiliary, covariantly conserved energy-momentum tensor with no internal degrees of freedom. We derive the generalized Einstein equations for these states and show that a homogeneous and isotropic initial background state contributes to expansion identical to cold dark matter. The inhomogeneous components of this state could source curvature perturbations that grow linearly at linear order. This auxiliary contribution to Einstein's equations could have either sign and thus provide a trivial way to violate the null energy condition, enabling novel gravitational dynamics such as cosmic bounces and wormholes.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Adiabatic quantum imaginary time evolution

We introduce an adiabatic state preparation protocol which implements quantum imaginary time evolution under the Hamiltonian of the system. Unlike the original quantum imaginary time evolution algorithm, adiabatic quantum imaginary time evolution does not require quantum state tomography during its runtime and, unlike standard adiabatic state preparation, the final Hamiltonian is not the system Hamiltonian. Instead, the algorithm obtains the adiabatic Hamiltonian by integrating a classical differential equation that ensures that one follows the imaginary time evolution state trajectory. We introduce some heuristics that allow this protocol to be implemented on quantum architectures with limited resources. We explore the performance of this algorithm via classical simulations in a one-dimensional spin model and highlight essential features that determine its cost, performance, and implementability for longer times, and compare to the original quantum imaginary time evolution for ground-state preparation. More generally, our algorithm expands the range of states accessible to adiabatic state preparation methods beyond those that are expressed as ground states of simple explicit Hamiltonians. Published by the American Physical Society 2024

Hejazi, Kasra (ORCID:000000032349478X)↗
DOE OSTI2021

Prehydrodynamic evolution and its signatures in final-state heavy-ion observables

We investigate the effects of prehydrodynamic evolution on final-state observables in heavy-ion collisions using state-of-the art event simulations coupled to different prehydrodynamic scenarios, which include the recently developed effective kinetic transport theory evolution model KøMPøST. Differential flow observables are found to be mostly insensitive to the details of prehydrodynamic evolution. The main effect we observe is in the p T spectra, particularly the mean transverse momentum. However, at least part of this effect is a consequence of the underlying conformal invariance assumption currently present in such approaches, which is known to be violated in the temperature regime probed in heavy-ion collisions. This assumption of early time conformal invariance leads to an artificially large out-of-equilibrium bulk pressure when switching from (conformal) prehydrodynamic evolution to hydrodynamics (using the nonconformal QCD equation of state), which in turn increases the transverse momentum. Our study indicates that a consistent treatment of prehydrodynamic evolution in heavy-ion collisions requires the use of nonconformal models of early time dynamics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Quadrupole collectivity in the neutron-rich sulfur isotopes 38,40,42,44 S

Electromagnetic transition strengths in the even-even neutron-rich sulfur isotopes 38,40,42,44 S were measured using intermediate-energy Coulomb excitation at the National Superconducting Cyclotron Laboratory. By utilizing the sensitivity of the experimental technique to E2 excitations from the ground state, the evolution of the pattern of B(E2) strengths to several low-lying 2 + states was investigated at Z = 16 from near stability to the N = 28 island of inversion. The experimental results allowed a detailed comparison with predictions from shell-model calculations using the SDPF-MU Hamiltonian, which was designed to describe collectivity in this region of the nuclear chart. While the shell-model calculations succeeded in modeling transition strengths at N = 22, 24, 26, the experimental B(E2; $0$ $^{+}_{1}$ → $2$ $^{+}_{1}$) at N = 28 was smaller than the predicted value by about a factor of 2, similar to previous observations for chlorine and argon isotopes around N = 28. The dependence of this overprediction by theory on the choice of effective charges was explored.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Chemical state of nickel nanoparticles during the oxygen evolution reaction in a carbonate-bicarbonate buffer solution

The chemical state of nickel anodes during the oxygen evolution reaction can impact their electrocatalytic performance. Here, X-ray photoelectron and absorption spectroscopies reveal the chemical state of nickel nanoparticles under oxygen evolution reaction conditions in amildly alkaline carbonate-bicarbonate buffer solution. Ni 2+ and Ni 3+ species are observed at the reaction onset potential with a 7:4 ratio, with no remaining metallic nickel. These species include NiO, which increasingly converts to other Ni 2+ and Ni 3+ species once the potential is increased above the onset potential. Conversely, when a 20-nm-thick nickel film is used instead of nickel nanoparticles, a significant amount of metallic nickel remains in the inner layers. Nickel nanoparticles also undergo significant morphological and structural changes during the reaction, as evidenced by ex situ transmission electron microscopy. Amorphization of the nanoparticles is attributed to significant H 2 O incorporation, with the oxygen intensity increasing both in operando and ex situ measurements.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Evidence for Photoinduced Polaron Generation in a High Persistence Length Low Bandgap Conjugated Polymer in Solution

Using ultrafast time-resolved infrared (TRIR) spectroscopy, we studied the solution-phase excited-state structural evolution of an indacenodithiophene-co-benzothiadiazole polymer (C8-IDTBT). Following band gap excitation, the TRIR spectra reveal vibrational features that develop within 10 ps and decay over 4 ns. Using pulse radiolysis measurements, charge-modulation spectroscopy, and quantum-chemical calculations, the IR features are assigned to polaron pairs. Interestingly, these features appear on an evolving broad mid-IR electronic absorption background, with kinetics correlating with the formation and decay of the cationradical vibrational bands. A three-state kinetic model successfully reproduces the spectral evolution, revealing that the polaron and exciton populations exist in dynamic equilibrium on picosecond time scales, with time constants for exciton dissociation in the range of 3− 5 ps and polaron-to-exciton reformation between 20 and 100 ps, while both species decay to the ground state on much slower nanosecond time scales (∼1 ns), yielding a remarkably high polaron-generation efficiency, higher than 50%. These findings provide fundamental insights into intramolecular charge photogeneration mechanisms in conjugated polymers, demonstrating efficient bound-polaron formation in isolated polymer chains.

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

String breaking in the heavy quark limit with scalable circuits

Quantum simulations of non-Abelian gauge theories require efficient mappings onto quantum computers and practical state preparation and measurement procedures. A truncation of the Hilbert space of non-Abelian lattice gauge theories with matter in the heavy quark limit is developed. This truncation is applied to SU(2) lattice gauge theory in 1+1D to map the theory efficiently onto a quantum computer. Scalable variational circuits are found to prepare the vacuum and single meson states. It is also shown how these state preparation circuits can be used to perform measurements of the number of mesons produced during the system’s time evolution. A state with a single qq¯ pair is prepared on quantum hardware and the inelastic production of qq¯ pairs is observed using 104 qubits on IBM’s Heron quantum computer ibm_torino.

Ciavarella, Anthony N↗
DOE OSTI2023

Excited-State Dynamics during Primary C–I Homolysis in Acetyl Iodide Revealed by Ultrafast Core-Level Spectroscopy

In typical carbonyl-containing molecules, bond dissociation events follow initial excitation to $nπ_{C=O}$$^*$ states. However, in acetyl iodide, the iodine atom gives rise to electronic states with mixed $nπ_{C=O}$$^*$ and $nπ_{C–I}$$^*$ character, leading to complex excited-state dynamics, ultimately resulting in dissociation. Using ultrafast extreme ultraviolet (XUV) transient absorption spectroscopy and quantum chemical calculations, we present an investigation of the primary photodissociation dynamics of acetyl iodide via time-resolved spectroscopy of core-to-valence transitions of the I atom after 266 nm excitation. The probed I 4d-to-valence transitions show features that evolve on sub-100-fs time scales, reporting on excited-state wavepacket evolution during dissociation. These features subsequently evolve to yield spectral signatures corresponding to free iodine atoms in their spin–orbit ground and excited states with a branching ratio of 1.1:1 following dissociation of the C–I bond. Calculations of the valence excitation spectrum via equation-of-motion coupled cluster with single and double substitutions (EOM-CCSD) show that initial excited states are of spin-mixed character. From the initially pumped spin-mixed state, we use a combination of time-dependent density functional theory (TDDFT)-driven nonadiabatic ab initio molecular dynamics and EOM-CCSD calculations of the N$_{4,5}$ edge to reveal a sharp inflection point in the transient XUV signal that corresponds to rapid C–I homolysis. Here, by examining the molecular orbitals involved in the core-level excitations at and around this inflection point, we are able to piece together a detailed picture of C–I bond photolysis in which d → σ* transitions give way to d → p excitations as the bond dissociates. We also report theoretical predictions of short-lived, weak 4d → 5d transitions in acetyl iodide, validated by weak bleaching in the experimental transient XUV spectra. This joint experimental–theoretical effort has thus unraveled the detailed electronic structure and dynamics of a strongly spin–orbit coupled system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗