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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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

A Theory-Guided X-ray Absorption Spectroscopy Approach for Identifying Active Sites in Atomically Dispersed Transition-Metal Catalysts

Atomically dispersed supported metal catalysts offer new properties and the benefits of maximized metal accessibility and utilization. The characterization of these materials, however, remains challenging. Using atomically dispersed platinum supported on crystalline MgO (chosen for its well-defined bonding sites) as a prototypical example, we demonstrate in this work how systematic density functional theory calculations for assessing all the potentially stable platinum sites, combined with automated analysis of extended X-ray absorption fine structure (EXAFS) spectra, leads to unbiased identification of isolated, surface-enveloped platinum cations as the catalytic species for CO oxidation. The catalyst has been characterized by atomic-resolution imaging and EXAFS and high-energy resolution fluorescence detection X-ray absorption near edge spectroscopy. The proposed platinum sites are in agreement with experiment. This theory-guided workflow leads to rigorously determined structural models and provides a more detailed picture of the structure of the catalytically active site than what is currently possible with conventional EXAFS analyses. As this approach is efficient and agnostic to the metal, support, and catalytic reaction, we posit that it will be of broad interest to the materials characterization and catalysis communities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1984

Comparison of the X-ray observations of the AM Herculis objects to theory

The X-ray observations of the original AM Her objects (AM Her, VV Pup, EF Eri, and AN UMa are reexamined. The work differs from that carried out previously in that the observed X-ray spectral properties are compared to theoretical models calculated using a dipolar accretion geometry rather than a spherically symmetric one, and the observed X-ray light curves are compared to theoretical light curves calculated assuming that the X-ray sources are cataclysmic variable-like binaries which contain a strongly magnetic white dwarf. The added constraints offered by the light curve properties restrict the possible kinds of X-ray emission scenarios in some cases. For instance, it is found that the X-ray observations of AM Her can be self-consistently explained by accretion powered radiative shock models. Further, the observations cannot be self-consistently explained by conduction dominated models as has been suggested by previous workers.

Imamura, J. N.↗
DOE OSTI2022

X-ray absorption spectra of f-element complexes: insight from relativistic multiconfigurational wavefunction theory

X-ray absorption near edge structure (XANES) spectroscopy, coupled with ab initio calculations, has emerged as the state-of-the-art tool for elucidating the metal-ligand bonding in f-element complexes. Furthermore, this highlight presents recent efforts in calculating XANES spectra of lanthanide and actinide compounds with relativistic multiconfiguration wavefunction approaches that account for differences in donation bonding in the ground state (GS) versus a core-excited state (ES), multiplet effects, and spin-orbit-coupling. With the GS and ES wavefunctions available, including spin-orbit effects, an arsenal of chemical bonding tools that are popular among chemists can be applied to rationalize the observed intensities in terms of covalent bonding.

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

Putting all the X in one basket: Updated X-ray constraints on sub-GeV Dark Matter

Sub-GeV dark matter particles can annihilate or decay producing e ± pairs which upscatter the low-energy photon fields in the Galaxy and generate an X-ray emission (via the Inverse Compton effect). Here, using X-ray data from X MM -N EWTON , I NTEGRAL , N U S TAR and S UZAKU , we derive new constraints on this class of dark matter (DM). In the annihilation case, our new bounds are the strongest available for DM masses above 180 MeV, reaching $\langle$σv$\rangle$ ≲ 10 -28 cm 3 /s for m DM ≃ 1 GeV. In the decay case, our bounds are the strongest to date over a large fraction of the considered mass range, constraining τ ≳ 10 28 s for m DM ≃ 1 GeV and improving by up to 3 orders of magnitude upon existing limits.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Theory of x-ray photon correlation spectroscopy for multiscale flows

Complex multiscale flows associated with instabilities and turbulence are commonly induced under high-energy density (HED) conditions, but accurate measurement of their transport properties has been challenging. X-ray photon correlation spectroscopy (XPCS) with coherent x-ray sources can, in principle, probe material dynamics to infer transport properties using time autocorrelation of density fluctuations. Here we develop a theoretical framework for utilizing XPCS to study material diffusivity in multiscale flows. We extend single-scale shear flow theories to broadband flows using a multiscale analysis that captures shear and diffusion dynamics. Our theory is validated with simulated XPCS for Brownian particles advected in multiscale flows. We demonstrate the versatility of the method over several orders of magnitude in timescale using sequential-pulse XPCS, single-pulse x-ray speckle visibility spectroscopy (XSVS), and double-pulse XSVS.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
NASA NTRS1996

Light ion components of the galactic cosmic rays: Nuclear interactions and transport theory

Light nuclei are present in the primary galactic cosmic rays (GCR) and are produced in thick targets due to projectile or target fragmentation from both nucleon and heavy induced reactions. In the primary GCR, He-4 is the most abundant nucleus after H-1. However, there are also a substantial fluxes of H-2 and He-3. In this paper we describe theoretical models based on quantum multiple scattering theory for the description of light ion nuclear interactions. The energy dependence of the light ion fragmentation cross section is considered with comparisons of inclusive yields and secondary momentum distributions to experiments described. We also analyze the importance of a fast component of lights ions from proton and neutron induced target fragementation. These theoretical models have been incorporated into the cosmic ray transport code HZETRN and will be used to analyze the role of shielding materials in modulating the production and the energy spectrum of light ions.

Cucinotta, F. A.↗
DOE OSTI2026

Insights on carbon dioxide adsorption in a flexible 1-D coordination polymer from in situ X-ray scattering and density functional theory

A combination of in situ small-angle X-ray scattering (SAXS) microstructure characterization over scales ranging from 1 nm to 10 µm and powder X-ray diffraction (XRD) structure characterization under various gas/pressure/temperature conditions with density functional theory (DFT) calculations provides new insights for the CO2 sorption behavior of a one-dimensional porous coordination polymer: catena-bis­(di­benzoyl­methanato)(4,4′-bi­pyridyl)­nickel(II), denoted NiDBM-Bpy. The NiDBM-Bpy chains are held together by van der Waals forces, but the structure of guest-free NiDBM-Bpy is unsolved due to a lack of suitable crystals and high-quality powder XRD patterns. Nevertheless, SAXS and powder XRD can follow microstructural and structural changes as a function of gas pressure, composition and temperature. Both mixed-gas flow and static supercritical CO2 regimes are explored experimentally. DFT calculations are used to model the structural variation associated with XRD changes and hysteresis in the sorption isotherms. XRD and DFT calculations suggest that an orthorhombic Fddd structure with two CO2 per Ni emerges following a transition from the structure with lower molar volume and symmetry that exists without CO2 present.

Allen, Andrew J.↗
NASA NTRS1981

Stellar and solar X-ray polarimetry

The theory of Bragg crystal X-ray polarimeters is presented together with an analysis of the statistics of photon-limited polarimeters. The focusing Bragg crystal polarimeter flown on the OSO-8 Satellite is described and a number of results obtained at 2.6 keV and 5.2 keV are presented. A polarimeter of this type with at least ten times the area is needed to answer a number of astrophysically interesting questions. A discussion is given of a Compton scattering polarimeter that is expected to be useful of energies above 40 keV. It is shown how this polarimeter may be used to test for the presence of a black hole in Cyg X-1. A solar flare X-ray polarimeter that is scheduled to be flown on an early space shuttle mission is described and an estimate is given of its sensitivity.

Novick, R.↗
NASA NTRS1976

Solar modulation and a galactic origin for the anomalous component observed in low-energy cosmic rays

The current theory of solar modulation can be used to argue that the cosmic-ray component at low energies, which is observed to have an anomalous composition, is not of galactic origin, i.e., it is not a component of the galactic cosmic-ray flux. The current theory predicts, from quite general considerations, that an unreasonably large intensity of cosmic rays, by many orders of magnitude, would be required in the interstellar medium to account for the observed fluxes. Conceivably, the current modulation theory could be modified so that only reasonable interstellar fluxes are predicted. One such modification involves an unusual scheme for particle diffusion in the interplanetary medium. Particles are assumed to diffuse not as a result of their own motion among small-scale irregularities in the magnetic field, but rather in a process in which they are trapped between time-varying constrictions in the large-scale field.

Fisk, L. A.↗
NASA NTRS1985

Magnetic fluctuation and cosmic ray diurnal variations

A unified theory of cosmic ray diurnal variations has been proposed in which the first 3 harmonics of the cosmic ray daily variation all results from a single anisotropy produced by the combined effects of adiabatic focusing and anisotropic pitch angle scattering. The theoretical description of steady state cosmic ray anisotropies are simplified and improved. Preliminary results of a study of correlations between cosmic ray diurnal variations and the fluctuation characteristics of the interplanetary magnetic field are presented and discussed in light of the theory.

Bieber, J. W.↗
DOE OSTI2023

Rigorous Oxidation State Assignments for Supported Ga-Containing Catalysts Using Theory-Informed X-ray Absorption Spectroscopy Signatures from Well-Defined Ga(I) and Ga(III) Compounds

Gallium-based heterogeneous catalysts originally developed for commercial use in propane dehydroaromatization have been explored extensively as potential replacements for Pt- and Cr-based catalysts used in propane dehydrogenation for on-demand propylene production. In a large number of experimental and theoretical studies, active sites with a variety of Ga nuclearities, coordination environments, and oxidation states have been proposed. Isolated Ga(I) ions are often invoked, despite the scarcity of well-defined molecular species and their well-documented instability. In this study, we investigate the appearance of a high-intensity, low-energy white line at the Ga K-edge upon reduction of Ga/HZSM-5 by H 2 at a temperature of ca. 500 °C, accompanied by a dramatic reduction in the extended X-ray absorption fine structure (EXAFS) intensity. In contrast, Ga/γ-Al 2 O 3 does not show such behavior. In order to lay a rigorous foundation for characterizing these types of systems and to establish experimental signatures for the elusive Ga(I) oxidation state, we recorded Ga K-edge X-ray absorption spectra [including high-energy-resolution fluorescence detection-X-ray absorption near-edge spectroscopy (HERFD-XANES)] for several well-defined molecular and crystalline Ga(I) compounds. XANES is essential to establishing the presence of Ga(I), despite the overlap in edge energies with organoGa(III) compounds, because Ga(I)-containing oxide materials show very weak EXAFS scattering. Compared to the XANES of trigonal Ga(III)-containing materials, Ga(I) spectra display a significantly more intense white line feature. Theoretical simulations agree well with this experimental observation and reveal that the strong XANES intensity originates from the superposition of transitions to several empty, nearly degenerate p-like states. Finally, these signatures provide compelling evidence for assigning the intense white line and dramatic loss of EXAFS intensity in Ga/HZSM-5 to the near-quantitative reduction of Ga(III) to Ga(I), while the weaker white line and conventional EXAFS signal of Ga/γ-Al 2 O 3 point to, at most, a minor fraction of Ga(I) sites.

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

The Reactivity and Structural Dynamics of Supported Metal Nanoclusters Using Electron Microscopy, in-situ X-Ray Spectroscopy, Electronic Structure Theories, and Molecular Dynamics Simulations

This research will provide new methods to determine the structures and compositions of heterogeneous catalysts as they exist in reaction conditions. The new tools will make it possible to understand how extremely small material structures—ones in a size range spanning from single atoms to larger polyatomic clusters—make it possible to carry out highly selective chemical transformations required to synthesize useful materials as well as for efficient energy production and utilization. The tools will make it possible to see how the atomic structures of catalytic materials evolve over time under the conditions of their use, and in this way provide understandings to guide the design of new energy-efficient catalysts. The work will make it possible to answer long standing questions that include the following. How does catalyst structure help guide molecules along specific reaction pathways? What are the important intermediates involved in these transformations? How do the structures and reactivity of catalytic materials, as well as the chemistry of their interfaces, vary with reaction conditions? Is it possible to develop new catalytic materials using new knowledge of the active structures and reaction mechanisms? The work will provide heretofore unavailable experimental tools that can be applied in advanced programs of research addressing such questions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗