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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

Measurements of nonequilibrium interatomic forces using time-domain x-ray scattering

Here, we demonstrate an experimental approach to determining the excited-state interatomic forces using femtosecond x-ray pulses from an x-ray free-electron laser. We determine experimentally the excited-state interatomic forces that connect photoexcited carriers to the nonequilibrium lattice dynamics in the prototypical Peierls-distorted material, bismuth. The forces are obtained by a constrained least-squares fit of a pairwise interatomic force model to the excited-state phonon dispersion relation as measured by the time- and momentum-resolved x-ray diffuse scattering. We find that photoexcited carriers weaken predominantly the nearest-neighbor forces, which drives the measured softening of the transverse acoustic modes throughout the Brillouin zone as well as the zone-center A 1g optical mode. This demonstrates a bond-selective approach to measuring electron-phonon coupling relevant to a broad range of photoinduced phase transitions and transient light-driven states in quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Revealing pressure-driven structural transitions in the hybrid improper ferroelectric Sr 3 Sn 2 O 7

In this work, we combine diamond anvil cell techniques and synchrotron-based infrared spectroscopy with a detailed symmetry analysis and lattice dynamics calculations to uncover a series of pressure induced structural phase transitions in the hybrid improper ferroelectric Sr 3 Sn 2 O 7 . The microscopic character of each high pressure phase is determined by comparing the measured spectrum with the predicted vibrational patterns of several related but distinct candidate space groups. Our analysis reveals a sequence of compression-induced transitions from A2 1 am ↔ Pnab ↔ Acaa ↔ I4/mmm at room temperature. Remarkably, this space group progression matches the sequence of temperature-dependent structural transitions observed in Sr 3 Sn 2 O 7 between 77 and 1000 K. Other hybrid improper ferroelectrics display a similar set of transitions, suggesting that pressure and probably strain will be very effective tuning parameters for this entire class of materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Optically and thermally driven huge lattice orbital and spin angular momenta from spinning fullerenes

Lattice vibration in solids may carry angular momentum. But unlike the intrinsic spin of electrons, the lattice vibration is rarely rotational. To induce angular momentum, one needs to find a material that can accommodate a twisted normal mode, two orthogonal modes, or excitation of magnons. If excitation is too strong, one may exceed the Lindemann limit, so the material melts. Therefore these methods are not ideal. Here, we theoretically propose a route to phonon angular momentum in a molecular crystal C 60 . We find that a single laser pulse is able to inject a significant amount of angular momentum to C 60 , and the momentum transfer is helicity dependent. Changing from right-circularly polarized light to left-circularly polarized light switches the direction of phonon angular momentum. On the ultrafast timescale, the orbital angular momentum change closely resembles the displacive excitation of coherent phonons, with a cosine-function dependence on time, different from the spin counterpart. Atomic displacements, even under strong laser excitation, remain far below the Lindemann criterion. Under thermal excitation, spinning C 60 even at room temperature generates a huge angular momentum close to several hundred h¯. Our finding opens the door to a large group of fullerenes, from C 60 , C 70 to their endohedral derivatives, where angular momentum can be generated through light or temperature. Furthermore, this paves the way to the phononic control electronic spin and harvesting thermal energy through phonon angular momentum.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Nonperturbative study of bulk photovoltaic effect enhanced by an optically induced phase transition

Solid systems with strong correlations and interactions under light illumination have the potential for exhibiting interesting bulk photovoltaic behavior in the non-perturbative regime, which has remained largely unexplored in the past theoretical studies. We investigate the bulk photovoltaic response of a perovskite manganite with strongly coupled electron-spin-lattice dynamics, using real-time simulations performed with a tight-binding model. The transient changes in the band structure and the photoinduced phase transitions, emerging from spin and phonon dynamics, result in a nonlinear current versus intensity behavior beyond the perturbative limit. The current rises sharply across a photoinduced magnetic phase transition, which later saturates at higher light intensities due to excited phonon and spin modes. The predicted peak photoresponsivity is orders of magnitude higher than other known ferroelectric oxides such as BiFeO$_3$. We disentangle phonon-and spin-assisted components to the ballistic photocurrent, showing that they are comparable in magnitude. Our results illustrate a promising alternative way for controlling and optimizing the bulk photovoltaic response through the photoinduced phase transitions in strongly-correlated systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Pressure-induced creation and annihilation of Weyl points in T d - Mo 0.5 W 0.5 Te 2 and 1 T " - Mo 0.5 W 0.5 Te 2

By means of first-principles density-functional theory calculations, we investigate the role of hydrostatic pressure in the electronic structure of the T d (Pmn2 1 ) and 1T" (Pm) phases of the Weyl semimetal Mo 0.5 W 0.5 Te 2 , which is a promising material for phase-change memory technology and superconductivity. We particularly focus on changes occurring in the distribution of the gapless Weyl points (WPs) within the 0 to 45 GPa pressure range. Here we further investigate the structural phase transition and lattice dynamics of the T d and 1T" phases within the aforementioned pressure range. Our calculations suggest that both the T d and 1T" phases of Mo 0.5 W 0.5 Te 2 host four WPs in their full Brillouin zone at zero pressure. The total number of WPs increases to 44 (36) with increasing pressure via pair creation up to 20 (15) GPa for the T d (1T") phase, and beyond this pressure pair annihilation of WPs starts occurring, leaving only 16 WPs at 45 GPa in both phases. The enthalpy versus pressure data reveal that the 1T" phase is more favorable below the critical pressure of 7.5 GPa; however, beyond this critical pressure the T d phase becomes enthalpically favorable. We also provide the calculated x-ray diffraction spectra along with the calculated Raman- and infrared-active phonon frequencies to facilitate the experimental identification of the studied phases

36 MATERIALS SCIENCE↗
DOE OSTI2022

Perturbation theory and thermal transport in mass-disordered alloys: Insights from Green's function methods

Lowest-order quantum perturbation theory (Fermi's golden rule) for phonon-disorder scattering has been used to predict thermal conductivities in several semiconducting alloys with surprising success given its underlying hypothesis of weak and dilute disorder. In this paper, we explain how this is possible by focusing on the case of maximally mass-disordered Mg 2 Si 1-x Sn x . In this work, we use a Chebyshev polynomials Green's function method, which allows a full treatment of disorder on very large systems (tens of millions of atoms) to probe individual phonon linewidths and frequency-resolved thermal transport. We demonstrate that the success of perturbation theory originates from the specific form of mass disorder terms in the phonon Green's function and from the interplay between anharmonic and disorder scattering.

36 MATERIALS SCIENCE↗
DOE OSTI2023

(2+1)-dimensional compact Lifshitz theory, tensor gauge theory, and fractons

The (2+1)-dimensional continuum Lifshitz theory of a free compact scalar field plays a prominent role in a variety of quantum systems in condensed matter physics and high energy physics. It is known that in compact space, it has an infinite ground-state degeneracy. In order to understand this theory better, we consider two candidate lattice regularizations of it using the modified Villain formalism. We show that these two lattice theories have significantly different global symmetries (including a dipole global symmetry), anomalies, ground-state degeneracies, and dualities. In particular, one of them is self-dual. Given these theories and their global symmetries, we can couple them to corresponding gauge theories. Here, these are two different U(1) tensor gauge theories. The resulting models have excitations with restricted mobility, i.e., fractons. Finally, we give an exact lattice realization of the fracton and lineon-elasticity dualities for the Lifshitz theory, and scalar and vector charge gauge theories.

2-dimensional systems↗
DOE OSTI2020

Microscopic Mechanisms of Glasslike Lattice Thermal Transport in Cubic Cu 12 Sb 4 S 13 Tetrahedrites

Materials based on cubic tetrahedrites (Cu 12 Sb 4 S 13 ) are useful thermoelectrics with unusual thermal and electrical transport properties, such as very low and nearly temperature-independent lattice thermal conductivity (κ L ). We explain the microscopic origin of the glasslike κ L in Cu 12 Sb 4 S 13 by explicitly treating anharmonicity up to quartic terms for both phonon energies and phonon scattering rates. We show that the strongly unstable phonon modes associated with trigonally coordinated Cu atoms are anharmonically stabilized above approximately 100 K and continue hardening with increasing temperature in accord with experimental data. This temperature-induced hardening effect reduces scattering of heat carrying acoustic modes by reducing the available phase space for three-phonon processes, thereby balancing the conventional ∝ T increase in scattering due to phonon population and yielding nearly temperature independent κ L . Furthermore, we find that very strong phonon broadening leads to a qualitative breakdown of the conventional phonon-gas model and modify the dominant heat transport mechanism from the particlelike phonon wave packet propagation to incoherent contributions described by the off-diagonal terms in the heat-flux operator, which are typically prevailing in glasses and disordered crystals. Furthermore, our work paves the way to a deeper understanding of glasslike thermal conductivity in complex crystals with strong anharmonicity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Breaking Rayleigh’s Law with Spatially Correlated Disorder to Control Phonon Transport

Controlling thermal transport in insulators and semiconductors is crucial for many technological fields such as thermoelectrics and thermal insulation, for which a low thermal conductivity (κ) is desirable. A major obstacle for realizing low κ materials is Rayleigh’s law, which implies that acoustic phonons, which carry most of the heat, are insensitive to scattering by point defects at low energy. We demonstrate, with large scale simulations on tens of millions of atoms, that isotropic long-range spatial correlations in the defect distribution can dramatically reduce phonon lifetimes of important low-frequency heat-carrying modes, leading to a large reduction of κ—potentially an order of magnitude at room temperature. We propose a general and quantitative framework for controlling thermal transport in complex functional materials through structural spatial correlations, and we establish the optimal functional form of spatial correlations that minimize κ. Finally, we end by briefly discussing experimental realizations of various correlated structures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Universal L - 3 finite-size effects in the viscoelasticity of amorphous systems

We present a theory of viscoelasticity of amorphous media, which takes into account the effects of confinement along one of three spatial dimensions. The framework is based on the nonaffine extension of lattice dynamics to amorphous systems, or nonaffine response theory. The size effects due to the confinement are taken into account via the nonaffine part of the shear storage modulus G'. The nonaffine contribution is written as a sum over modes in k-space. With a rigorous argument based on the analysis of the k-space integral over modes, it is shown that the confinement size L in one spatial dimension, e.g., the z axis, leads to a infrared cutoff for the modes contributing to the nonaffine (softening) correction to the modulus that scales as L -3 . Corrections for finite sample size D in the two perpendicular dimensions scale as ~(L/D) 4 , and are negligible for L«D. For liquids it is predicted that G'~L -3 is in agreement with a previous more approximate analysis, whereas for amorphous materials G'~G' bulk +βL -3 . For the case of liquids, four different experimental systems are shown to be very well described by the L-3 law. The theory can also explain previous simulation data of confined jammed granular packings.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Interplay of 𝑑- and 𝑝-states in RbTi3⁢Bi5 and CsTi3⁢Bi5 flat-band kagome metals

Shifting the Fermi level of the celebrated 𝐴⁢𝑀3⁢𝑋5 (135) compounds into proximity of flat bands strongly enhances electronic correlations and severely affects the formation of density waves and superconductivity. Our broadband infrared spectroscopy measurements of RbTi3⁢Bi5 and CsTi3⁢Bi5 combined with density-functional band-structure calculations reveal that the correlated Ti 𝑑-states are intricately coupled with the Bi 𝑝-states that form a tilted Dirac crossing. Electron-phonon coupling manifests itself in the strong damping of itinerant carriers and in the anomalous shape of the phonon line in RbTi3⁢Bi5. An anomaly in these spectral features around 150 K can be paralleled to the onset of nematicity detected by low-temperature probes. Our findings show that the materials with low band filling open unexplored directions in the physics of kagome metals and involve electronic states of different nature strongly coupled with lattice dynamics.

Wenzel, Matthew [ORNL]↗
DOE OSTI2020

High-energy-resolution inelastic X-ray scattering spectrometer at beamline 30-ID of the Advanced Photon Source

Inelastic X-ray scattering is a powerful and versatile technique for studying lattice dynamics in materials of scientific and technological importance. In this article, the design and capabilities of the momentum-resolved high-energy-resolution inelastic X-ray spectrometer (HERIX) at beamline 30-ID of the Advanced Photon Source are reported. The instrument operates at 23.724 keV and has an energy resolution of 1.3–1.7 meV. It can accommodate momentum transfers of up to 72 nm -1 , at a typical X-ray flux of 4.5 × 10 9 photons s -1 meV -1 at the sample. A suite of in situ sample environments are provided, including high pressure, static magnetic fields and uniaxial strains, all at high or cryogenic temperatures.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Giant isotope effect on phonon dispersion and thermal conductivity in methylammonium lead iodide

Lead halide perovskites are strong candidates for high-performance low-cost photovoltaics, light emission, and detection applications. A hot-phonon bottleneck effect significantly extends the cooling time of hot charge carriers, which thermalize through carrier–optic phonon scattering, followed by optic phonon decay to acoustic phonons and finally thermal conduction. To understand these processes, we adjust the lattice dynamics independently of electronics by changing isotopes. We show that doubling the mass of hydrogen in methylammonium lead iodide by replacing protons with deuterons causes a large 20 to 50% softening of the longitudinal acoustic phonons near zone boundaries, reduces thermal conductivity by ~50%, and slows carrier relaxation kinetics. Phonon softening is attributed to anticrossing with the slowed libration modes of the deuterated molecules and the reduced thermal conductivity to lowered phonon velocities. Our results reveal how tuning the organic molecule dynamics enables control of phonons important to thermal conductivity and the hot-phonon bottleneck.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Thermal Neutron Scattering Law Evaluation for Zirconium Carbide and Critical Mass Calculations

Zirconium carbide (ZrC) is a candidate material for use in advanced high temperature reactors, including space nuclear thermal propulsion applications. Thermal neutron scattering laws (TSLs) are generated for carbon bound in ZrC, C(ZrC), and zirconium bound in ZrC, Zr(ZrC), using ab initio lattice dynamics methods. These evaluations are to be submitted for inclusion in ENDF/B-VIII.1 and use the incoherent approximation for inelastic scattering as well as the new mixed elastic scattering treatment. The application of disordered alloy theory is introduced to appropriately capture the isotopic composition of Zr and C in the elastic scattering cross section. Localized higher energy vibrations in the C(ZrC) phonon density of states that are separated from lower energy modes result in quantized oscillations in the inelastic contributions to the TSL with a significant likelihood of large energy down-scattering and up-scattering interactions, where the latter increases in probability with temperature. The quanta of energy transfer during neutron thermalization is substantially greater than classically expected within the thermal neutron energy range. MC21 critical mass calculations of ZrC mixtures with high-enriched uranium demonstrate an impact of the TSLs when compared to free-gas treatment for 235 U concentrations less than 0.2 g/cm 3 . Additional MC21 critical mass calculations with homogenous mixtures of ZrC and reactor-grade graphite also demonstrate sensitivity to the ZrC TSL for thermal spectrum driven fission systems.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Hard x-ray – optical four-wave mixing using a split-and-delay line

New, hard x-ray free electron lasers (FEL) produce intense femtosecond-to-attosecond pulses at angstrom wavelengths, giving access to the fundamental spatial and temporal scales of matter. These revolutionary light sources open the door to applying the suite of nonlinear, optical spectroscopy methods at hard x-ray photon energies. Nonlinear spectroscopy with hard x-rays can allow for measuring the coherence properties of short wavelength excitations with atomic specificity and for understanding how high energy excitations couple to other degrees of freedom in atomic, molecular or condensed-phase systems. As a step in this direction, here we present hard x-ray, optical four-wave mixing (4WM) measurements done at 9.8 keV at the split-and-delay line at the x-ray correlation spectroscopy (XCS) hutch of the Linac Coherent Light Source (LCLS). In this work, we create an x-ray transient grating (TG) from a pair of crossing x-ray beams and diffract optical laser pulses at 400 nm from the TG. The key technical advance here is being able to independently vary the delays of the x-ray pulses. Measurements were made in 3 different solid samples: bismuth germinate (BGO), zinc oxide (ZnO) and yttrium aluminum garnet (YAG). The resulting phase-matched, 4WM signal is measured in two different ways: by varying the x-ray, x-ray pulse delay which can reveal both material and light source coherence properties and also by varying the optical laser delay with respect to the x-ray TG to study how the x-ray excitation couples to the optical properties. Although no coherent 4WM signal was seen in these measurements, the absence of this signal gives important information on experimental requirements for detecting this in future work. Also, our laser-delay scans, although not a new measurement, were applied to different materials than in past work and reveal new examples x-ray induced lattice dynamics in solids. This work represents a key step towards extending nonlinear optics and time-resolved spectroscopy into the hard x-ray regime.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

First-Principles Thermodynamic Assessments of Sr-Containing Secondary Phase Formation in La1-xSrxMnO3±δ Perovskites for Solid Oxide Cell Applications

Sr-secondary phase formation is a potentially significant degradation mode threatening solid-oxide cell (SOC) commercial viability. A first-principles thermodynamic study was performed for rhombohedral perovskite (La1-xSrx) MnO3±δ (LSM) to assess its stability against Sr secondary phase formation in SOC applications. In this work, the Sr secondary phase formation reaction free energies were determined by combining ab initio lattice dynamics calculations for the solid phases and an ab initio thermodynamics approach for the gas phases. Furthermore, this approach goes beyond previous thermodynamic modeling studies by integrating first-principles based point-defect equilibria into the analyses. The modeling results indicate an increased tendency to form SrO oxide from LSM upon decreasing the oxygen partial pressure. Additionally, enhancing factors to form the Sr-related secondary phase from the associated SrO activity in LSM are further quantified by considering the equilibrium of SrO reacting with contaminant gas species as a function of temperature and gas pressure.

Defect and phase stability↗
DOE OSTI2025

Novel Superionic Na Conductors for Solid‐State Na batteries: Materials and Interface

This project aims to advance the fundamental understanding on how the cation or anion doping influence on the crystal structure, phase stability and ion transport of novel Na superionic conductors. Specifically, we focus on the Na 3-x A x SbS 4-y X y family solid electrolytes (A: cation dopant, X: anion dopant), a class of promising materials for all-solid-state sodium batteries owing to their high ionic conductivity and compositional tunability. By integrating materials synthesis, neutron scattering, and electrochemical characterization and theoretical simulations, this project sees to elucidate 1) how does the synthesis approaches (solid-state reaction, low-temperature reaction) on the phase purity and doping process; 2) how chemical doping (A: cation dopants such as Sn; X: anion dopants such as Se, F) modulate lattice dynamics and Na+ migration as well as interface stability toward Na metal. Specifically, this project’s proposed technology involves three objectives: (1) synthesize novel Na-ion conductors (anion or cation doped Na 3 SbS 4 ) with high phase purity and examine their structural features (e.g., phase stability); (2) understand Na-ion conductive properties of new Na-ion conductors through a combination of experimental characterizations and theoretical simulations; (3) investigate the interface stability of novel Na superionic conductors with electrode materials in solid-state Na batteries. These objectives will be achieved through combined experimental synthesis/characterizations and computational approaches. The obtained knowledge will provide a comprehensive synthesis-structure-property correlation, enabling the rational design of novel solid-state conductors with excellent conductivity and stability.

25 ENERGY STORAGE↗
DOE OSTI2022

Unexpected features in the optical vibrational spectra of δ-UO 3

Uranium trioxide displays a complex chemical phase space, with at least six structurally distinct polymorphs accessible via different synthetic routes. Remarkably, despite its technological importance, full structural and electronic characterization of these polymorphs remains an open area of study. δ-UO 3 in particular has attracted significant theoretical attention due to its high point group and space group symmetries, having U (VI) in octahedral coordination with polyhedra interconnected through corner-sharing to build a 3-D cubic lattice with space group symmetry Pm-3m and Z = 1. Critical experimental information, such as its optical vibrational spectra, are not known. Here, we study the Raman and infrared (IR) spectra of δ-UO 3 together with the support of density functional theory (DFT) calculations for spectral interpretation. A symmetry analysis of the DFT-predicted phonon eigenmodes indicates that δ-UO 3 should have two IR active modes and no Raman active modes. Experimental results, however, indicate significant Raman scattering from δ-UO 3 . We therefore propose four potential explanations for this apparent contradiction: a possible tetragonal distortion to the cubic cell, the existence of a surface impurity layer, vacancy scattering, and structural activation of Raman signal. We use powder X-ray diffraction and confocal Raman spectroscopy with depth profiling to investigate these possibilities and suggest future experiments to explore this phenomenon in more detail. Understanding the lattice dynamics of δ-UO 3 is important for identification of technogenic U phases via Raman and infrared spectroscopy and our results indicate that the simple understanding of δ-UO 3 as a high-symmetry cubic structure should be reconsidered.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗