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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 OSTI2021

Deep Optical Switching on Subpicosecond Timescales in an Amorphous Ge Metamaterial

Active nanostructured optical components show promise as potential building blocks for novel light-based computing and data processing architectures. However, nanoscale all-optical switches that have low activation powers and high-contrast ultrafast switching have been elusive so far. Here, pump–probe measurements performed on amorphous-Ge-based micro-resonator metasurfaces that exhibit strong resonant modes in the mid-infrared are reported. Relative change is observed in transmittance of ΔT/T ≈ 1 with picosecond (down to τ ≈ 0.5 ps) free carrier relaxation rates, obtained with very low pump fluences of 50 μJ cm –2 . In this work, these observations are attributed to efficient free carrier promotion, affecting light transmittance via high quality-factor optical resonances, followed by an increased electron–phonon scattering of free carriers due to the amorphous crystal structure of Ge. Full-wave simulations based on a permittivity model that describes free-carrier damping through crystal structure disorder find excellent agreement with the experimental data. These findings offer an efficient and robust platform for all-optical switching at the nanoscale.

36 MATERIALS SCIENCE↗
DOE OSTI2023

High-Temperature Thermodynamics of Uranium from Ab Initio Modeling

We present high-temperature thermodynamic properties for uranium in its γ phase (γ-U) from first-principles, relativistic, and anharmonic theory. The results are compared to CALPHAD modeling. The ab initio electronic structure is obtained from density-functional theory (DFT) that includes spin–orbit coupling and an added self-consistent orbital-polarization (OP) mechanism for more accurate treatment of magnetism. The first-principles method is coupled to a lattice dynamics scheme that is used to model anharmonic lattice vibrations, namely, Self-Consistent Ab Initio Lattice Dynamics (SCAILD). The methodology can be summarized in the acronym DFT + OP + SCAILD. Upon thermal expansion, γ-U develops non-negligible magnetic moments that are included for the first time in thermodynamic theory. The all-electron DFT approach is shown to model γ-U better than the commonly used pseudopotential method. In addition to CALPHAD, DFT + OP + SCAILD thermodynamic properties are compared with other ab initio and semiempirical modeling and experiments. Our first-principles approach produces Gibbs free energy that is essentially identical to CALPHAD. The DFT + OP + SCAILD heat capacity is close to CALPHAD and most experimental data and is predicted to have a significant thermal dependence due to the electronic contribution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Startup regime of high-efficiency tapering-enhanced FEL oscillator

In this paper, we present a design of a high-efficiency high-gain free-electron laser oscillator based on the use of a strongly tapered undulator for extracting energy from high-brightness electron beams. We provide an analytical model of the setup followed by numerical simulations for lasing at the wavelength of 13.5 nm. We discuss the optimization of the system in steady state and the conditions necessary for the pass-per-pass buildup of the power from shot noise level. We propose the use of fast phase shifters as a way to accelerate the buildup. Finally, we present time-dependent simulations of the oscillator and discuss the role of spectral filtering. The optimized working point yields a total energy conversion efficiency from the electron beam to output radiation above 1% at the wavelength of 13.5 nm.

Beam dynamics↗
DOE OSTI2023

CLASSY. VI. The Density, Structure, and Size of Absorption-line Outflows in Starburst Galaxies

Galaxy formation and evolution are regulated by the feedback from galactic winds. Absorption lines provide the most widely available probe of winds. However, since most data only provide information integrated along the line of sight, they do not directly constrain the radial structure of the outflows. In this paper, we present a method to directly measure the gas electron density in outflows (n e ), which in turn yields estimates of outflow cloud properties (e.g., density, volume filling factor, and sizes/masses). We also estimate the distance (r n ) from the starburst at which the observed densities are found. We focus on 22 local star-forming galaxies primarily from the COS Legacy Archive Spectroscopic SurveY (CLASSY). In half of them, we detect absorption lines from fine-structure excited transitions of Si $\tiny{II}$ (i.e., Si $\tiny{II}$ * ). We determine n e from relative column densities of Si $\tiny{II}$ and Si $\tiny{II}$ * , given Si $\tiny{II}$ * originates from collisional excitation by free electrons. We find that the derived n e correlates well with the galaxy's star formation rate per unit area. From photoionization models or assuming the outflow is in pressure equilibrium with the wind fluid, we get r n ~ 1–2r * or ~5r * , respectively, where r * is the starburst radius. Based on comparisons to theoretical models of multiphase outflows, nearly all of the outflows have cloud sizes large enough for the clouds to survive their interaction with the hot wind fluid. Most of these measurements are the first ever for galactic winds detected in absorption lines and, thus, will provide important constraints for future models of galactic winds.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Electrocatalytic Reduction of CO 2 to CO over Ag(110) and Cu(211) Modeled by Grand-Canonical Density Functional Theory

We report the results of modeling CO 2 reduction (CO 2 R) to CO over Ag(110) and Cu(211) surfaces at different applied potentials using grand-canonical density functional theory (GC-DFT), a method specifically designed to accurately model electrochemical systems. In addition to demonstrating GC-DFT’s ability to accurately model electrochemical processes, we also compare it with the computational hydrogen electrode (CHE) approach. GC-DFT predicts that the geometries of these reacting systems strongly depend on the applied potential and the Helmholtz free energies vary nonlinearly with the applied potential, which contradicts a central assumption of the CHE approach. The CHE approach neglects the change in the number of electrons on the electrode surface at different applied potentials, which reduces its accuracy as the potential changes from the potential of zero charge. Our results further demonstrate that the grand free energies of the reaction intermediates not only depend on the value of the applied potential but also on the metal surface type, adsorption site, and adsorbate. GC-DFT’s ability to predict the effect of the applied potential on adsorbate geometry enables it to evaluate different possible reaction mechanisms at different applied potentials. For instance, GC-DFT predicts that the first step of CO2R likely switches from proton-coupled electron transfer to sequential electron transfer and then proton transfer at more reducing potentials, a result that cannot be determined by the CHE because it assumes that all electron transfers are coupled to proton transfers and neglects the effect of the applied potential on the adsorbate geometry.

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

Machine learning-guided design of direct methanol fuel cells with a platinum group metal-free cathode

Direct methanol fuel cells (DMFCs) offer a promising solution for clean electricity generation, particularly in small electronics and remote auxiliary power units. However, optimizing their efficiency and performance is challenging due to the complex interactions between various factors. Here, we present a novel approach that integrates experiments with machine learning to model and predict the performance of these fuel cells using atomically dispersed platinum group metal (PGM)-free catalysts at the cathode. Further, our machine learning models, trained on diverse input parameters, allow for the comprehensive optimization of DMFC performance prior to fabrication and testing. Through extensive experimental validation, we demonstrate that this data-driven approach accurately predicts key performance metrics, such as maximum power output and polarization curves. By combining our models with interpretable game-theory methods, we provide deep insights into the factors governing fuel cell performance, ultimately paving the way for the design of scalable and efficient DMFC technologies.

25 ENERGY STORAGE↗
DOE OSTI2020

Machine learning a molecular Hamiltonian for predicting electron dynamics

We develop a computational method to learn a molecular Hamiltonian matrix from matrix-valued time series of the electron density. As we demonstrate for three small molecules, the resulting Hamiltonians can be used for electron density evolution, producing highly accurate results even when propagating 1,000 time steps beyond the training data. As a more rigorous test, we use the learned Hamiltonians to simulate electron dynamics in the presence of an applied electric field, extrapolating to a problem that is beyond the field-free training data. We find that the resulting electron dynamics predicted by our learned Hamiltonian are in close quantitative agreement with the ground truth. Our method relies on combining a reduced-dimensional, linear statistical model of the Hamiltonian with a time-discretization of the quantum Liouville equation within time-dependent Hartree Fock theory. In conclusion, we train the model using a least-squares solver, avoiding numerous, CPU-intensive optimization steps. For both field-free and field-on problems, we quantify training and propagation errors, highlighting areas for future development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Simulation and flow physics of a shocked and reshocked high-energy-density mixing layer

This work describes a computational investigation of multimode instability growth and multimaterial mixing induced by multiple shock waves in a high-energy-density (HED) environment, where pressures exceed 1 Mbar. The simulations are based on a series of experiments performed at the National Ignition Facility (NIF) and designed as an HED analogue of non-HED shock-tube studies of the Richtmyer–Meshkov instability and turbulent mixing. A three-dimensional computational modelling framework is presented. It treats many complications absent from canonical non-HED shock-tube flows, including distinct ion and free-electron internal energies, non-ideal equations of state, radiation transport and plasma-state mass diffusivities, viscosities and thermal conductivities. The simulations are tuned to the available NIF data, and traditional statistical quantities of turbulence are analysed. Integrated measures of turbulent kinetic energy and enstrophy both increase by over an order of magnitude due to reshock. Large contributions to enstrophy production during reshock are seen from both the baroclinic source and enstrophy–dilatation terms, highlighting the significance of fluid compressibility in the HED regime. Dimensional analysis reveals that Reynolds numbers and diffusive Péclet numbers in the HED flow are similar to those in a canonical non-HED analogue, but conductive Péclet numbers are much smaller in the HED flow due to efficient thermal conduction by free electrons. It is shown that the mechanism of electron thermal conduction significantly softens local spanwise gradients of both temperature and density, which causes a minor but non-negligible decrease in enstrophy production and small-scale mixing relative to a flow without this mechanism.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Carrier properties of Bi(111) grown on mica and Si(111)

A comparison is presented between properties of Bi(111) films grown by Stranski-Krastanov epitaxy on Si(111) 7 × 7 and by van der Waals epitaxy on mica substrates. Thin film morphologies and electronic transport properties of Bi(111) films of variable thickness are investigated for each growth method. Atomic force micrographs for Bi(111) films on mica reveal clearly defined triangular regions consisting of layered steps with height 0.4 nm, corresponding to the Bi(111) bilayer height. Variable-temperature electronic transport measurements show the existence of a quantum confinement-induced energy gap in the film interiors, resulting in a semimetal-to-semiconductor transition. Magnetotransport analysis in a three-carrier model including metallic electrons in surface states and electrons and holes in the films' interiors provides a detailed study of densities, mobilities, and mean-free paths of the three carrier types. Further, improved electronic transport properties are found in Bi(111) films of higher thickness on mica compared to on Si(111), a likely result of the largely strain-free van der Waals epitaxial growth.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Bridging the gap of storage ring light sources and linac-driven free-electron lasers

High-gain free-electron lasers (FELs) are driven by short, high-charge density electron beams as only produced at dedicated single pass or recirculating linear accelerators. We describe new conceptual, technical, and modeling solutions to produce subpicosecond, up to ~100 μJ-energy extreme ultra-violet and soft x-ray FEL pulses at high- and tunable repetition rates, from diffraction-limited storage ring light source. In contrast to previously proposed schemes, we show that lasing can be simultaneous to the standard multibunch radiation emission from short insertion devices, and that it can be obtained with limited impact on the storage ring infrastructure. By virtue of the high-average power but moderate pulse energy, the storage ring-driven high-gain FEL would open the door to unprecedented accuracy in time-resolved spectroscopic analysis of matter in the linear response regime, in addition to inelastic scattering experiments.

43 PARTICLE ACCELERATORS↗
DOE OSTI2023

Band Energy Dependence of Defect Formation in the Topological Semimetal Cd3As2

Cadmium Arsenide (Cd3As2) is a prototypical Dirac semimetal that manifests topological properties in a 3D bulk material. In defect-free Cd3As2, the Fermi level lies at a minimum in the density of states at the Dirac point, but experimentally it forms with excess electron carriers and an elevated EF, thereby masking the topological features. To computationally study the self-doping of Cd3As2, we combine density functional theory (DFT) calculations for defect formation energies with quasi-particle self-consistent GW (QSGW) electronic structure calculations. We demonstrate an innate dependence of the point defect formation energies on carrier concentrations and use the QSGW calculated density of states to extrapolate formation energies to arbitrary electron concentrations. This approach allows the quantitative modeling of thermodynamic defect equilibria in topological semimetals and is used to predict how Cd3As2 growth conditions affect the position of EF relative to the Dirac point.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS↗
DOE OSTI2020

Chromium isotope fractionation during reduction of Chromium(VI) by Iron(II/III)-bearing clay minerals

Chromium stable isotope ratios are used to trace the reduction of Cr(VI) to Cr(III) in both ancient and modern systems. However, quantitative interpretation of Cr isotopic signatures has been stymied by the large variability in isotopic fractionation factors for Cr(VI) reduction by different reductants. Here we determine Cr isotope fractionation factors during Cr(VI) reduction by Fe(II/III)-bearing clay minerals, which are abundant in subsurface environments. Several variables were tested: pH, total Fe content of the clay, and the fraction of reduced Fe within the clay (Fe(II)/Fe(total)). The latter controls the standard reduction potential of the clay. Our results demonstrate that neither pH nor total Fe content of the clay have major effects on isotopic fractionation. In contrast, as the effective standard reduction potential of the clay and thus the standard free energy of Cr(VI) reduction become more negative, Cr isotope fractionation factors decrease in magnitude from - 4.9 to -1.3‰ according to a linear free energy relationship. This linear free energy relationship can be predicted from Marcus electron transfer theory and allows first-order predictions of Cr isotope fractionation factors to be made from the standard reduction potential or Fe(II)/Fe(total) of a clay, potentially improving our ability to model Cr isotope signatures in geochemical systems. Chromium is the first isotope system to show such a linear free energy relationship over a diverse range of reductants, including both aqueous and solid-phase reductants, and may provide a model for determining other redox-driven kinetic isotope effects in environmentally important isotope systems.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Octahedral Distortion and Excitonic Behavior of Cs 3 Bi 2 Br 9 Halide Perovskite at Low Temperature

The metal halide ionic octahedron, represented as [MX 6 ] $n$- (M = metal cation, X = halide anion), serves as the basic structural unit in halide perovskites and plays a crucial role in determining their optoelectronic and chemical properties. Thus, it is possible to correlate the responses of metal halide perovskites to various environmental stimuli with the dynamic behaviors of the [MX 6 ] $n$- octahedra. In this study, with the temperature-dependent single-crystal X ray diffraction (SCXRD) measurements on Cs 3 Bi 2 Br 9 2D halide perovskites, we can identify two classes of distortions through the lowering of temperature: intraoctahedral distortion, which is the off-centering of Bi 3+ cation within a [BiBr 6 ] 3– octahedron due to the Bi 3+ 6s 2 lone pair electrons, and interoctahedral distortion, which is the collective misalignments among the [BiBr 6 ] 3– building blocks. Free exciton (FE) and self-trapped exciton (STE) models are used to study the relationship between the distortion of octahedra in Cs 3 Bi 2 Br 9 and the corresponding changes in its optoelectronic properties, which transform from dominating blue emission above 100 K to red emission at 4 K. In conclusion, this work provides new insights into the excitonic behaviors of perovskites and suggests a possibility that we can design and rationalize the optical properties of halide perovskites by regulating the environmental stimuli based on the knowledge of behaviors of the individual [MX 6 ] $n$- building blocks.

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

Spectral deconvolution without the deconvolution: Extracting temperature from x-ray Thomson scattering spectra without the source-and-instrument function

X-ray Thomson scattering (XRTS) probes the dynamic structure factor of the system, but the measured spectrum is broadened by the combined source-and-instrument function (SIF) of the setup. In order to extract properties such as temperature from an XRTS spectrum, the broadening by the SIF needs to be removed. Recent work [Dornheim et al. Nat. Commun. 13 , 7911 (2022)] has suggested that the SIF may be deconvolved using the two-sided Laplace transform. However, the extracted information can depend strongly on the shape of the input SIF, and the SIF is in practice challenging to measure accurately. Here, we propose an alternative approach: we demonstrate that considering ratios of Laplace-transformed XRTS spectra collected at different scattering angles is equivalent to performing the deconvolution, but without the need for explicit knowledge of the SIF. From these ratios, it is possible to directly extract the temperature from the scattering spectra, when the system is in thermal equilibrium. We find the method to be generally robust to spectral noise and physical differences between the spectrometers, and we explore situations in which the method breaks down. Furthermore, the fact that consistent temperatures can be extracted for systems in thermal equilibrium indicates that non-equilibrium effects could be identified by inconsistent temperatures of a few eV between the ratios of three or more scattering angles.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Ionic Dopant-Induced Ordering Enhances the Thermoelectric Properties of a Polythiophene-Based Block Copolymer

Conjugated polymer-based block copolymers (CP-BCPs) are an unexplored class of materials for organic thermoelectrics. In this study, the authors report on the electronic conductivity (σ) and Seebeck coefficient (α) of a newly synthesized CP-BCP, poly(3-hexylthiophene)-block-poly (oligo-oxyethylene methacrylate) (P3HT-b-POEM), upon solution co-processing with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and subsequently vapor-doping with a molecular dopant, 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ). It is found that the addition of the hydrophilic block POEM greatly enhances the processability of P3HT, enabling homogeneous solution-mixing with LiTFSI. Notably, interactions between P3HT-b-POEM with ionic species significantly improve molecular order and unexpectedly cause electrical oxidizing doping of P3HT block both in solution and solid-states, a phenomenon that has not been previously observed in Li-salt containing P3HT. Vapor doping of P3HT-b-POEM-LiTFSI thin films with F4TCNQ further enhances σ and yields a thermoelectric power factor PF = α 2 σ of 13.0 μW m -1 K -2 , which is more than 20 times higher than salt-free P3HT-b-POEM sample. Through modeling thermoelectric behaviors of P3HT-b-POEM with the Kang-Snyder transport model, the improvement in PF is attributed to higher electronic charge mobility originating from the enhanced molecular ordering of P3HT. The results demonstrate that solution co-processing CP-BCPs with a salt is a powerful method to control structure and performance of organic thermoelectric materials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Stochastic modeling of x-ray superfluorescence

An approach to modeling the dynamics of x-ray amplified spontaneous emission and superfluorescence, the phenomenon of collective x-ray emission initiated by intense pulses of x-ray free-electron lasers, is developed based on stochastic partial differential equations. The equations are derived from first principles, and the relevant approximations, derivation steps, and extensions specific to stimulated x-ray emission are presented. The resulting equations take the form of three-dimensional generalized Maxwell-Bloch equations augmented with noise terms for both field and atomic variables. The derived noise terms possess specific correlation properties that enable the correct reconstruction of spontaneous emission. Consequently, the developed theoretical formalism is universally suitable for describing all stages of stimulated x-ray emission: spontaneous emission, amplified spontaneous emission, and superfluorescence. Here, we present numerical examples that illustrate various properties of the emitted field, including spatiotemporal coherence and spectral-angular and polarization characteristics. We anticipate that the proposed theoretical framework will establish a robust foundation for interpreting measurements in stimulated x-ray emission spectroscopy, modeling x-ray laser oscillators, and describing other experiments leveraging x-ray superfluorescence.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Platform for probing radiation transport properties of hydrogen at conditions found in the deep interiors of red dwarfs

We describe an experimental concept at the National Ignition Facility for specifically tailored spherical implosions to compress hydrogen to extreme densities (up to ∼800× solid density, electron number density ne∼4×1025 cm−3) at moderate temperatures (T∼200 eV), i.e., to conditions, which are relevant to the interiors of red dwarf stars. The dense plasma will be probed by laser-generated x-ray radiation of different photon energy to determine the plasma opacity due to collisional (free–free) absorption and Thomson scattering. The obtained results will benchmark radiation transport models, which in the case for free–free absorption show strong deviations at conditions relevant to red dwarfs. This very first experimental test of free–free opacity models at these extreme states will help to constrain where inside those celestial objects energy transport is dominated by radiation or convection. Moreover, our study will inform models for other important processes in dense plasmas, which are based on electron–ion collisions, e.g., stopping of swift ions or electron–ion temperature relaxation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Toward direct spatial and intensity characterization of ultra-high-intensity laser pulses using ponderomotive scattering of free electrons

Spatial distributions of electrons ionized and scattered from ultra-low-pressure gases are proposed and experimentally demonstrated as a method to directly measure the intensity of an ultra-high-intensity laser pulse. Analytic models relating the peak scattered electron energy to the peak laser intensity are derived and compared to paraxial Runge–Kutta simulations highlighting two models suitable for describing electrons scattered from weakly paraxial beams (f#>5) for intensities in the range of 1018−1021 W cm−2. Scattering energies are shown to be dependent on gas species, emphasizing the need for specific gases for given intensity ranges. Direct measurements of the laser intensity at full power of two laser systems are demonstrated, both showing a good agreement between indirect methods of intensity measurement and the proposed method. One experiment exhibited the role of spatial aberrations in the scattered electron distribution, motivating a qualitative study on the effect. We propose the use of convolutional neural networks as a method for extracting quantitative information on the spatial structure of the laser at full power. We believe the presented technique to be a powerful tool that can be immediately implemented in many high-power laser facilities worldwide.

47 OTHER INSTRUMENTATION↗