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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 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Photothermal behaviour of titanium nitride nanoparticles evaluated by transient X-ray diffraction

The photothermal properties of metal nitrides have recently received significant attention owing to diverse applications in solar energy conversion, photothermal therapies, photoreactions, and thermochromic windows. Here, the photothermal response of titanium nitride nanoparticles is examined using transient X-ray diffraction, in which optical excitation is synchronized with X-ray pulses to characterize dynamic changes in the TiN lattice. Photoinduced diffraction data is quantitatively analyzed to determine increases in the TiN lattice spacing, which are furthermore calibrated against static, temperature-dependent diffraction patterns of the same samples. Measurements of 20 nm and 50 nm diameter TiN nanoparticles reveal transient lattice heating from room temperature up to similar to 175 degrees C for the highest pump fluences investigated here. Increasing excitation intensity drives sublinear increases in lattice temperature, due to increased heat capacity at the higher effective temperatures achieved at higher powers. Temporal dynamics show that higher excitation intensity drives not only higher lattice temperatures, but also unexpectedly slower cooling of the TiN nanoparticles, which is attributed to heating of the solvent proximal to the nanoparticle surface.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction

The ultrafast laser excitation of matters leads to nonequilibrium states with complex solid-liquid phase-transition dynamics. In this paper, we used electron diffraction at mega–electron volt energies to visualize the ultrafast melting of gold on the atomic scale length. For energy densities approaching the irreversible melting regime, we first observed heterogeneous melting on time scales of 100 to 1000 picoseconds, transitioning to homogeneous melting that occurs catastrophically within 10 to 20 picoseconds at higher energy densities. We showed evidence for the heterogeneous coexistence of solid and liquid. We determined the ion and electron temperature evolution and found superheated conditions. Finally, our results constrain the electron-ion coupling rate, determine the Debye temperature, and reveal the melting sensitivity to nucleation seeds.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Tracking dissociation pathways of nitrobenzene via mega-electron-volt ultrafast electron diffraction

As the simplest nitroaromatic compound, nitrobenzene is an interesting model system to explore the rich photochemistry of nitroaromatic compounds. Previous investigations of nitrobenzene's photochemical dynamics have probed structural and electronic properties. These investigations paint, at times, a convoluted and sometimes contradictory description of the photochemical landscape. Here, we investigate the ultrafast dynamics of nitrobenzene triggered by photoexcitation at 267 nm for the first time using a structural probe with femtosecond time resolution. Our probe complements previous measurements of nitrobenzene's electronic structure evolution and aids in determining the photochemical dynamics with less ambiguity. We employ megaelectronvolt ultrafast electron diffraction to follow nitrobenzene's structural evolution within the first 5 ps after photoexcitation. We observe ground state recovery within 160 ± 60 fs through nonadiabatic dynamics. Based on comparisons of the experimental signal with molecular dynamics simulations, we exclude a significant population of the triplet manifold. Furthermore, we do not observe fragmentation of nitrobenzene within the investigated time window, which indicates that previously observed photofragmentation reactions take place in the vibrationally 'hot' ground state on timescales considerably beyond 5 ps.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Melting and solidification dynamics during laser melting of reaction-based metal matrix composites uncovered by in-situ synchrotron X-ray diffraction

Laser additive manufacturing (AM) of reaction-based metal matrix composites (MMCs) involves highly complex and non-equilibrium material transformation behavior, including melting, dissolution, precipitation, and solidification. Yet, the dynamics and interplay of these phase transformation processes remain poorly understood, posing substantial challenges in identifying the microstructure formation mechanism, and predicting and controlling the microstructure in the printed parts. Here, in this study, we performed the in-situ X-ray diffraction experiment to characterize the phase evolution dynamics of the 316L + 10 vol.%TiC system during laser melting, which provides direct and quantitative insights of the complex phase reaction and evolution dynamics under rapid heating and cooling conditions relevant to additive manufacturing of reaction-based MMCs. Further in-depth thermodynamic and kinetic calculations revealed that most of the phase evolution behavior observed in the in-situ X-ray diffraction experiment cannot be solely explained by widely used equilibrium thermodynamic models, and diffusion-controlled nonequilibrium dissolution and precipitation kinetics must be considered to elucidate the complex phase evolution behavior, including incomplete TiC dissolution, and three-step TiC precipitation. The three distinct types of precipitates generate unique hierarchical TiC micro- and nanostructures, which enhances the yield strength from 513 MPa to 877 MPa by 71 %, tensile strength from 628 MPa to 1054 MPa by 68 %, and Young's modulus from 193 GPa to 221 GPa by 14 %. The findings of our research provide the knowledge foundation for the design of unique microstructures and advanced MMC materials through laser AM.

36 MATERIALS SCIENCE↗
DOE OSTI2026

BMINN: Learning chemical potentials and parameters from voltage data for multi-phase battery modeling

Free-energy landscapes and chemical potentials govern the dynamics of phase transitions, transport, and stability in functional materials, yet they remain experimentally inaccessible under realistic operating conditions. Here we introduce a Bayesian model-integrated neural network (BMINN) that embeds physics-based formulations of non-autonomous partial differential-algebraic equations into probabilistic learning. This approach reconstructs hidden thermodynamics directly from macroscopic current-voltage data, providing quantitative access to metastable states, staging transitions, and energy barriers without synchrotron probes. Demonstrated on lithium-graphite electrodes, BMINN recovers full Gibbs free-energy landscapes with fidelity validated against operando X-ray diffraction. The framework generalizes across dynamical regimes, enabling accurate voltage prediction, internal state estimation, and inference of governing parameters. Beyond batteries, BMINN exemplifies a broadly applicable strategy for learning missing physics in multiphase, non-equilibrium systems, offering a new pathway to uncover hidden thermodynamic functions across condensed matter and materials physics.

25 ENERGY STORAGE↗
DOE OSTI2022

Intermolecular correlations of liquid and glassy CS 2 studied by synchrotron radiation x-ray diffraction

How is the orientation of molecular liquids ordered on cooling? What are the basic structures of molecular glasses, e.g., close to the crystalline structure or some special structures such as icosahedral cluster? These are long-standing questions in liquid and glass physics. Here, we have constructed a novel cryostat to prepare simple molecular glasses by vapor deposition and performed in situ synchrotron radiation x-ray diffraction experiments. The glassy state of a simple molecule CS 2 , which cannot be vitrified by normal liquid quenching, was successfully prepared with this instrument, and its diffraction data were collected in a wide Q-range of 0.16–25.7 Å -1 with a high-energy diffractometer at BL04B2, SPring-8. The diffraction data of liquid CS 2 were also recorded in a wide temperature range of 160–300 K. These diffraction data were analyzed with molecular dynamics simulations and reverse Monte Carlo modelings to investigate orientational correlation. From the obtained 3D structure models, the orientational correlation between neighboring CS 2 molecules was investigated quantitatively as a function of temperature. At room temperature, the parallel and T-shaped arrangements are preferred for the nearest neighbor correlation. On cooling, these arrangements are developed gradually, and its rate became prominent below the melting temperature (162 K). In the glassy state, the slipped-parallel arrangement is dominant as well as the T-shaped arrangement. Both arrangements appear in the CS 2 crystal, indicating that the structure of glassy CS 2 is close to that of crystalline CS 2 .

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

Nonstereotypical Distribution and Effect of Ergosterol in Lipid Membranes

Ergosterol, found in fungi and some protist membranes, is understudied compared with cholesterol from animal membranes. Generally, ergosterol is assumed to modulate membranes in the same manner as cholesterol, based on their similar chemical structures. Here we reveal some fundamental structural and dynamical differences between them. Neutron diffraction shows that ergosterol is embedded in the lipid bilayer much shallower than cholesterol. Further, ergosterol does not change the membrane thickness as much as cholesterol does, indicating little condensation effect. Neutron spin echo shows that ergosterol can rigidify and soften membranes at different concentrations. The lateral lipid diffusion measured by quasielastic neutron scattering indicates that ergosterol promotes a jump diffusion of the lipid, whereas cholesterol keeps the same continuous lateral diffusion as the pure lipid membrane. Our results point to quite distinct interactions of ergosterol with membranes compared with cholesterol. These insights provide a basic understanding of membranes containing ergosterol with implications for phenomena such as lipid rafts and drug interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Demonstration of femtosecond X-ray pump X-ray probe diffraction on protein crystals

The development of X-ray free-electron lasers (XFELs) has opened the possibility to investigate the ultrafast dynamics of biomacromolecules using X-ray diffraction. Whereas an increasing number of structures solved by means of serial femtosecond crystallography at XFELs is available, the effect of radiation damage on protein crystals during ultrafast exposures has remained an open question. We used a split-and-delay line based on diffractive X-ray optics at the Linac Coherent Light Source XFEL to investigate the time dependence of X-ray radiation damage to lysozyme crystals. For these tests, crystals were delivered to the X-ray beam using a fixed-target approach. The presented experiments provide probe signals at eight different delay times between 19 and 213 femtoseconds after a single pump event, thereby covering the time-scales relevant for femtosecond serial crystallography. Even though significant impact on the crystals was observed at long time scales after exposure with a single X-ray pulse, the collected diffraction data did not show significant signal reduction that could be assigned to beam damage on the crystals in the sampled time window and resolution range. This observation is in agreement with estimations of the applied radiation dose, which in our experiment was clearly below the values expected to cause damage on the femtosecond time scale. The experiments presented here demonstrate the feasibility of time-resolved pump-multiprobe X-ray diffraction experiments on protein crystals.

43 PARTICLE ACCELERATORS↗
NASA NTRS1998

Lattice Dynamics of Colloidal Crystals During Photopolymerization of Acrylic Monomer Matrix

The photoinitiated bulk polymerization process, which has been used recently in the manufacture of solid optical diffraction filters, is examined to understand the dynamics of both the crystalline colloidal arrays (CCA) and the host monomer species. Our analysis indicates that volume shrinkage of the monomer, changes in the dielectric properties of the monomer, and inhomogeneities of polymerization reaction rate across the dispersion during the polymerization process, are the major contributors for observed lattice compression and lattice disorder of the CCA of silica spheres in polymerized acrylic/methacrylic ester films. The effect of orientation of photocell with respect to the radiation source on Bragg diffraction of CCA indicated the presence of convective stirring in the thin fluid system during the photopolymerization that deleteriously affects the periodic array structures. To devise reproducible and more efficient optical filters, experimental methods to minimize or eliminate convective instabilities in monomeric dispersions during polymerization are suggested.

Sunkara, H. B,↗
DOE OSTI2024

In situ visualisation of zeolite anisotropic framework flexibility during catalysis

Zeolites exhibit framework flexibility driving their chemical and catalytic properties. Since the zeolitic pores are extremely small, a slight strain generated in the crystal induces compelling changes in shape, connectivity, accessibility, and the framework chemical properties. These modifications affected the adsorption and desorption of reactants/products and the diffusion within the channels during reaction. Using in situ 3D Bragg coherent X-ray diffraction imaging, we unveil the dynamics of the zeolite structure during catalysis, contraction and/or expansion of its framework also known as zeolite framework flexibility. Here, we imaged three-dimensionally a single faujasite zeolite crystal during the ethanol dehydration reaction revealing anisotropic lattice dynamics simultaneously to guest molecules formation. Understanding zeolite flexibility could permit to tune zeolites properties towards potentially higher adsorption and selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Dynamics of Electron–Phonon Coupling in Bicontinuous Nanoporous Gold

Here, the nanosize effect on electron–phonon interactions in free-electron noble metals has been a subject of intense discussion because of their important applications in physics, chemistry, and biomedicine. However, the interference from supports of dispersive nanoparticulate metals has led to controversial observations. We utilize freestanding, bicontinuous nanoporous gold (NPG) films to investigate electron–phonon interaction dynamics using ultrafast MeV electron diffraction. Compared to solid gold films, NPG shows faster electron–phonon interaction and thus noticeably higher electron–phonon coupling constant. The results demonstrate that surface states of electrons and phonons play an important role in electron–phonon coupling of nanostructured materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Catalysis by Metal Organic Frameworks: Perspective and Suggestions for Future Research

Metal organic frameworks (MOFs) have drawn wide attention as potential catalysts, offering high densities of catalytic sites in high-area porous solids, some with stabilities at high temperatures. The field is at an early stage, characterized by numerous discoveries and novel demonstrations of catalytic properties associated with the crystalline structures of MOFs, but applications of MOFs as catalysts are still lacking. In this perspective we summarize advantages and limitations of MOFs as catalysts and fundamental issues to be addressed about their potential applications. MOF framework compositions and pore structures can strongly influence catalytic performance, allowing, for example, shape-selective and bifunctional catalysis, but research is needed to quantify reaction/transport processes in MOFs, identify catalytic sites, and determine intrinsic catalytic reaction rates. Progress is hindered by the lack of understanding of the heterogeneity of MOFs, with catalytic sites sometimes being in structures such as defects not determined by X-ray diffraction crystallography. Determination of the dynamics of MOFs and their catalytic sites, as well as the intrinsic kinetics of catalytic reactions, will help to advance guidelines for synthesizing optimum catalysts. Further, MOFs present challenges related to stability and regeneration as catalysts, some associated with the unique nature of MOFs, such as the node–linker bonds, which can break during catalysis. There are opportunities to understand these matters in depth and to find conditions of catalytic operation that minimize the processes leading to deactivation.

catalysis (heterogeneous), materials and chemistry↗
DOE OSTI2022

Low Thermal Conductivity in Heteroanionic Materials with Layers of Homoleptic Polyhedra

Although BiAgOSe, an analogue of a well-studied thermoelectric material BiCuOSe, is thermodynamically stable, its synthesis is complicated by the low driving force of formation from the stable binary and ternary intermediates. Here we have developed a “subtraction strategy” to suppress byproducts and produce pure phase BiAgOSe using hydrothermal methods. Electronic structure calculations and optical characterization show that BiAgOSe is an indirect bandgap semiconductor with a bandgap of 0.95 eV. The prepared sample exhibits lower lattice thermal conductivities (0.61 W·m –1 ·K –1 at room temperature and 0.35 W·m –1 ·K –1 at 650 K) than BiCuOSe. Further, lattice dynamical simulations and variable temperature diffraction measurements demonstrate that the low lattice thermal conductivity arises from both the low sound velocity and high phonon–phonon scattering rates in BiAgOSe. These in turn result primarily from the soft Ag–Se bonds in the edge-sharing AgSe 4 tetrahedra and large sublattice mismatch between the quasi-two-dimensional [Bi 2 O 2 ] 2+ and [Ag 2 Se 2 ] 2– layers. These results highlight the advantages of manipulating the chemistry of homoleptic polyhedra in heteroanionic compounds for electronic structure and phonon transport control.

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

Bidirectional phonon emission in two-dimensional heterostructures triggered by ultrafast charge transfer

Photoinduced charge transfer in van der Waals heterostructures occurs on the 100 fs timescale despite weak interlayer coupling and momentum mismatch. However, little is understood about the microscopic mechanism behind this ultrafast process and the role of the lattice in mediating it. Here, using femtosecond electron diffraction, we directly visualize lattice dynamics in photoexcited heterostructures of WSe 2 /WS 2 monolayers. Following the selective excitation of WSe 2 , we measure the concurrent heating of both WSe 2 and WS 2 on a picosecond timescale—an observation that is not explained by phonon transport across the interface. Using first-principles calculations, we identify a fast channel involving an electronic state hybridized across the heterostructure, enabling phonon-assisted interlayer transfer of photoexcited electrons. Phonons are emitted in both layers on the femtosecond timescale via this channel, consistent with the simultaneous lattice heating observed experimentally. Taken together, this shows our work indicates strong electron–phonon coupling via layer-hybridized electronic states—a novel route to control energy transport across atomic junctions.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Temperature-induced gradual polymorphic structural crossover in liquid indium, tin, and antimony

Temperature-induced polymorphic structural crossover in metallic liquid indium (In), tin (Sn), and antimony (Sb) is investigated by in situ high-energy x-ray diffraction and ab initio molecular dynamics simulations. The results demonstrate the existence of a temperature-induced reversible and gradual structural crossover in these three liquids, reflecting from both “static” structures, e.g., peak positions of the structure factor and pair distribution function, bond angle distribution, number of tetrahedra, cluster connection, free volume, and dynamical behaviors, including the relaxation time, diffusion coefficient, and non-Gaussian parameter. Further, the main difference from liquid In, Sn, to Sb is that not only the large-sized free volume but also the anharmonicity and the dynamical heterogeneity increase significantly with the appearance of strong covalent bonds. These findings will deepen the understanding of liquid structure and the liquid-liquid transition in metallic liquids.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Coupling of structure to magnetic and superconducting orders in quasi-one-dimensional K 2 Cr 3 As 3

Here, quasi-one-dimensional A 2 Cr 3 As 3 (with A = K, Cs, Rb) is an intriguing new family of superconductors which exhibit many similar features to the cuprate and iron-based unconventional superconductor families. Yet, in contrast to these systems, no charge or magnetic ordering has been observed which could provide the electronic correlations presumed necessary for an unconventional superconducting pairing mechanism—an absence which defies predictions of first-principles models. We report the results of neutron scattering experiments on polycrystalline K 2 Cr 3 As 3 (T c ~ 7) which probed the low-temperature dynamics near T c . Neutron diffraction data evidence a subtle response of the nuclear lattice to the onset of superconductivity while inelastic scattering reveals a highly dispersive column of intensity at the commensurate wave vector q = (001/2) which loses intensity beneath T c -indicative of short-range magnetic fluctuations. Using linear spin-wave theory, we model the observed scattering and suggest a possible structure to the short-range magnetic order. These observations suggest that K 2 Cr 3 As 3 is in close proximity to a magnetic instability and that the incipient magnetic order both couples strongly to the lattice and competes with superconductivity, in direct analogy with the iron-based superconductors.

1-dimensional systems↗
DOE OSTI2017

Surface buckling of black phosphorus: Determination, origin, and influence on electronic structure

The surface structure of black phosphorus materials is determined using surface-sensitive dynamical microspot low energy electron diffraction ( μ LEED ) analysis using a high spatial resolution low energy electron microscopy (LEEM) system. Samples of (i) crystalline cleaved black phosphorus (BP) at 300 K and (ii) exfoliated few-layer phosphorene (FLP) of about 10 nm thickness which were annealed at 573 K in vacuum were studied. In both samples, a significant surface buckling of 0.22 Å and 0.30 Å, respectively, is measured, which is one order of magnitude larger than previously reported. As direct evidence for large buckling, we observe a set of (for the flat surface forbidden) diffraction spots. Using first-principles calculations, we find that the presence of surface vacancies is responsible for the surface buckling in both BP and FLP, and is related to the intrinsic hole doping of phosphoresce materials previously reported.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗