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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 847 records · Page 47
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Autoionization resonances in the photoabsorption spectra of Fe{sup n+} iron ions

The photoabsorption cross sections of a neutral iron atom, as well as positive Fe{sup +} and Fe{sup 2+} ions, are calculated in the relativistic random-phase approximation with exchange in the energy range 20–160 eV. The wavefunctions of the ground and excited states are calculated in the single-configuration Hartree–Fock–Dirac approximation. The resultant photoabsorption spectra are compared with experimental data and with the results of calculations based on the nonrelativistic spin-polarized version of the random-phase approximation with exchange. Series of autoionization resonance peaks, as well as giant autoionization resonance lines corresponding to discrete transitions 3p → 3d, are clearly observed in the photoabsorption cross sections. The conformity of the positions of calculated peaks of giant autoionization resonances with experimental data is substantially improved by taking into account additionally the correlation electron–electron interaction based on the model of the dynamic polarization potential.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Bi-Kappa Proton Mirror and Cyclotron Instabilities in the Solar Wind

Abstract The charged particles in the solar wind are often observed to possess a nonthermal tail in the velocity distribution function, a feature that can be fitted with the Kappa model. The anisotropic, or bi-Kappa, model of protons, electrons, and other charged particles is thus adopted in the literature for interpreting the data as well as in the context of the analysis of wave–particle interactions. The present paper develops an approximate but efficient theory of the mirror and cyclotron instabilities excited by the bi-Kappa protons in the solar wind. A velocity moment-based quasi-linear theory of these instabilities is also formulated in order to investigate the saturation behavior. Applications of the formalism are made for instabilities close to the marginally unstable state, which is typical of the solar wind near 1 au.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2016

Correlation effects on spin-polarized electron-hole quantum bilayer

We present a numerical calculation for the intra- and interlayer pair-correlation functions, g{sub ll’}(r), of spin-polarized electron-hole quantum bilayers at zero temperature. The calculations of g{sub ll’}(r) are performed by including electron correlations within the dynamical version of the self-consistent mean-field approximation of Singwi, Tosi, Land and Sjölander (qSTLS). Our study reveals that the critical layer density decreases (increases) due to the inclusion of finite width (mass-asymmetry) effect during the phase-transition from charge-density wave to Wigner crystal ground-state by yielding the pronounced oscillatory behavior ing{sub ll}(r). The results are compared with recent findings of spin-polarized electron-hole quantum bilayers with mass-symmetry and zero width effects. To highlight the importance of dynamical character of correlations, we have also compared our results with the STLS results.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Mn- and N- doped carbon as promising catalysts for oxygen reduction reaction: Theoretical prediction and experimental validation

Development of platinum group metal (PGM)-free as well as iron-free electrocatalysts is imperative to achieve low-cost and long-term durability of polymer electrolyte membrane fuel cells. Here in this paper, we combined computational and experimental studies to investigate the mechanism, activity, and durability of Mn and N co-doped carbon (denoted as Mn-N-C) as promising catalysts for oxygen reduction reaction (ORR) in challenging acid medium. The first-principles density functional theory calculations predict that it is favorable for O 2 to be reduced into H 2 O via four-electron pathway on MnN 4 sites embedded in carbon layer. Using the reaction energies calculated from DFT, microkinetic analysis predicts that the MnN 4 sites could catalyze ORR with a half-wave potential only 60 mV lower than that of Pt (111) and 80 mV lower than that of the FeN 4 sites embedded in carbon layer, assuming the same density of active sites in the catalysts. Motivated by the computational prediction, we synthesized a Mn-N-C catalyst using a polymer (i.e., polyaniline-PANI) hydrogel precursors via a high temperature approach. Structural characterization indicates that atomically dispersed Mn sites coordinated with N are very likely formed in the catalyst. Electrochemical measurements show that the synthesized Mn-N-C catalyst can promote four-electron ORR with a catalytic activity in acids comparable to that of the Fe-N-C catalyst prepared using the same procedure. More importantly, the Mn-N-C catalyst exhibits superior potential cyclic stability, only losing 20 mV after 10000 cycles (0.6 to 1.0 V in O 2 saturated electrolyte). In comparison, the Fe-N-C catalyst would loss 80 mV after only 5000 cycles under the same testing conditions. Our computational and experimental results strongly suggest that the Mn and N co-doped carbon could be promising high-performance catalysts for ORR in acidic medium.

25 ENERGY STORAGE↗
DOE OSTI2023

Understanding the Uncertainty in the Technical Performance Level Assessment for Wave Energy

In recent years, the design and development of wave energy converters (WECs) has been explored with intense interest, with highly varying design concepts emerging globally across both research enterprises and industry. The design space for WECs is vast - many concepts ranging in functionality, control systems, power development systems, materials, and scale have been ideated and prototyped, but WEC technology has yet to converge. One critical element of the technology trajectory that governs the speed of adoption is the performance of a WEC concept. In analogous but more-established industries (such as aerospace, and environmentally sustainable electronics design), performance assessment is a quantitative method, based on historical data, that is used as an iterative tool to improve the design of these systems early on in the design process. Though more nascent than these approaches, in wave energy R&D, WEC performance has been assessed using the Technology Performance Level (TPL) assessment, which provides designers with a quantitative score, situating a grid-scale WEC concept on a scale from 1-9 (1 being the lowest performance, and 9 being the highest, trending with the oft-used Technology Readiness Level, or TRL). The TPL assessment is designed to be used during design iteration, when a WEC concept is fully ideated, to enable designers to consider potential means of improving the downstream performance of the concept. One concern that may be slowing the adoption of TPL among WEC developers is the inherent uncertainty in the assessment, and how uncertainty in the individual questions asked as part of the assessment may contribute to perceived inaccuracies in the final score. In this work, we explore the uncertainty present in the assessment and quantify this uncertainty using both traditional mathematical operations and a Monte Carlo simulation. Results imply areas of improvement of the TPL assessment, where reducing uncertainty will be most helpful to end users, enabling both TPL practitioners and users to understand with more accuracy those design elements that can be improved to impact device performance most substantively.

techno-economic analysis↗
DOE OSTI2021

Progress towards understanding ultranonlocality through the wave-vector and frequency dependence of approximate exchange-correlation kernels

In the framework of time-dependent density functional theory (TDDFT), the exact exchange-correlation (xc) kernel f xc (n, q, ω) determines the ground-state energy, excited-state energies, lifetimes, and the time-dependent linear density response of any many-electron system. The recently developed MCP07 xc kernel f xc (n, q, ω) of A. Ruzsinszky et al. [Phys. Rev. B 101, 245135 (2020)] yields excellent uniform electron gas (UEG) ground-state energies and plausible plasmon lifetimes. As MCP07 is constructed to describe f xc of the UEG, it cannot capture optical properties of real materials. To verify this claim, we follow Nazarov et al. [Phys. Rev. Lett. 102, 113001 (2009)] to construct the long-range, dynamic xc kernel, lim q→0 f xc (n, q, ω) = -α(ω)e 2 /q 2 , of a weakly inhomogeneous electron gas, using MCP07 and other common xc kernels. The strong wavevector and frequency dependence of the “ultranonlocality” coefficient α(ω) is demonstrated for a variety of simple metals and semiconductors. We examine how imposing exact constraints on an approximate kernel shapes α(ω). Comparisons to kernels derived from correlated-wavefunction calculations are drawn.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Computation of Auger Electron Spectra in Organic Molecules with Multiconfiguration Pair-Density Functional Theory

Efficient and accurate computation of molecular Auger electron spectra for larger systems is limited by the rapid increase in the number of doubly ionized final states as the system size grows. Here, in this work, we benchmark the application of multiconfiguration pair-density functional theory with a restricted active space (RAS) reference wave function for computing the carbon K-edge decay spectra of 20 organic molecules. Decay rates are computed within the one-center approximation. We evaluate the performance of different basis sets and on-top functionals and find that multiconfiguration pair-density functional theory achieves accuracy comparable to RAS followed by second-order perturbation theory, but at significantly lower computational cost.

Fouda, Adam E. A. [Argonne National Laboratory (AN↗
DOE OSTI2016

The dielectric function of weakly ionized dusty plasmas

Using classical Boltzmann kinetic theory, the dielectric function of weakly ionized unmagnetized dusty plasma is derived. The elastic Coulomb collision and inelastic charging collision of electrons with charged dust particle as well as charge variation on dust surface are taken into account. The theoretical result is applied to analyze the propagation of electromagnetic wave in a dusty plasma. It is demonstrated that the additional collision mechanism provided by charged dust particle can significantly increase the absorbed power of electromagnetic wave. These increases are mainly determined by the dust radius, density, and the charge numbers on the dust surface. The obtained results will support an enhanced understanding of the wave propagation processes in space and laboratory dusty plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Spinor $GW$ Bethe-Salpeter calculations in BerkeleyGW: Implementation, symmetries, benchmarking, and performance

Computing the GW quasiparticle band structure and Bethe-Salpeter equation (BSE) absorption spectra for materials with spin-orbit coupling have commonly been done by treating GW corrections and spin-orbit coupling (SOC) as separate perturbations to density-functional theory. However, accurate treatment of materials with strong spin-orbit coupling (such as many topological materials of recent interest, and thermoelectrics) often requires a nonperturbative approach using spinor wave functions in the Kohn-Sham equation and GW/BSE. Such calculations have only recently become available, in particular for the BSE. Here, we have implemented this approach in the plane-wave pseudopotential GW/BSE code BerkeleyGW, which is highly parallelized and widely used in the electronic-structure community. We present reference results for quasiparticle band structures and optical absorption spectra of solids with different strengths of spin-orbit coupling, including Si, Ge, GaAs, GaSb, CdSe, Au, and Bi 2 Se 3 . The calculated quasiparticle band gaps of these systems are found to agree with experiment to within a few tens of meV. SOC splittings are found to be generally in better agreement with experiment, including quasiparticle corrections to band energies. The absorption spectrum of GaAs is not significantly impacted by the inclusion of spin-orbit coupling due to its relatively small value (0.2 eV) in the Λ direction, while the absorption spectrum of GaSb calculated with the spinor GW/BSE captures the large spin-orbit splitting of peaks in the spectrum. For the prototypical topological insulator Bi 2 Se 3 , we find a drastic change in the low-energy band structure compared to that of DFT, with the spinorial treatment of the GW approximation correctly capturing the parabolic nature of the valence and conduction bands after including off-diagonal self-energy matrix elements. We present the detailed methodology, approach to spatial symmetries for spinors, comparison against other codes, and performance compared to spinless GW/BSE calculations and perturbative approaches to SOC. This work aims to spur further development of spinor GW/BSE methodology in excited-state research software and enables a more accurate and detailed exploration of electronic and optical properties of materials containing elements with large atomic numbers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Electronic structure and lattice dynamics of 1⁢𝑇−VSe 2 : Origin of the three-dimensional charge density wave

To characterize in detail the charge density wave (CDW) transition of 1⁢𝑇−VSe 2 , its electronic structure and lattice dynamics are comprehensively studied by means of x-ray diffraction, muon spectroscopy, angle resolved photoemission (ARPES), diffuse and inelastic x-ray scattering, and state-of-the-art first-principles density functional theory calculations. Resonant elastic x-ray scattering does not show any resonant enhancement at either V or Se, indicating that the CDW peak at the 𝐾 edges describes a purely structural modulation of the electronic ordering. ARPES experiments identify (i) a pseudogap at 𝑇 > 𝑇⁢ CDW , which leads to a depletion of the density of states in the ML-M'L' plane at 𝑇 < 𝑇⁢ CDW , and (ii) anomalies in the electronic dispersion reflecting a sizable impact of phonons on it. A diffuse scattering precursor, characteristic of soft phonons, is observed at room temperature (RT) and leads to the full collapse of the low-energy phonon (𝜔 1 ) with propagation vector (0.25 0 −0.3) r.l.u. Here, we show that the frequency and linewidth of this mode are anisotropic in momentum space, reflecting the momentum dependence of the electron-phonon interaction (EPI), hence demonstrating that the origin of the CDW is, to a much larger extent, due to the momentum dependent EPI with a small contribution from nesting. The pressure dependence of the 𝜔 1 soft mode remains nearly constant up to 13 GPa at RT, with only a modest softening before the transition to the high-pressure monoclinic C2/m phase. The wide set of experimental data is well captured by our state-of-the art first-principles anharmonic calculations with the inclusion of van der Waals corrections in the exchange-correlation functional. The comprehensive description of the electronic and dynamical properties of VSe 2 reported here adds important pieces of information to the understanding of the electronic modulations in the family of transition-metal dichalcogenides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Structural and optical characterization of dilute Bi-doped GaN nanostructures grown by molecular beam epitaxy

We have carried out detailed studies on the epitaxy and characterization of dilute Bi-doped GaN nanostructures. A comprehensive investigation of Bi-doped GaN nanowires and quasi-film epitaxial growth conditions has been performed. Scanning electron microscopy studies show that lowering the GaBiN growth temperature causes gradual changes in top c-plane nanowire morphology due to the incremental incorporation of foreign Bi atoms. This trend is further substantiated by the secondary ion mass spectroscopy analysis of a multi-layer Bi-doped GaN quasi-film. However, it is also found that the amount of Bi incorporation into the GaN lattice is relatively independent of the N2 flow rate variation under the growth conditions investigated. Furthermore, room-temperature micro-Raman spectra show that there are additional peaks near 530, 650, and 729 cm−1 wave numbers in the Bi-doped GaN samples, which can primarily be attributed to Bi local vibrational modes, indicative of a small amount of Bi incorporation in the GaN lattice. Moreover, phonon calculations with density functional theory indicate that Bi replacing the N sites is the likely origin of the experimentally measured Raman modes. X-ray photoelectron spectroscopy measurements have also been obtained to deduce the electronic interaction between the Bi dopant atom and the GaN nanostructure. Such one-dimensional nanowires permit the synthesis of dislocation-free highly mismatched alloys due to strain relaxation, allowing efficient light absorption and charge carrier extraction that is relevant for solar energy harvesting and artificial photosynthesis.

Materials Science↗
DOE OSTI2026

Effects of a magnetic field on hot electron generation from laser-plasma instabilities

We performed two-dimensional simulations of turbulent laser-plasma instabilities in the presence and absence of external magnetic fields using the Laser Plasma Simulation Environment (LPSE) code. The results demonstrate that, in the presence of a magnetic field, the transition from ballistic to gyrating electron motion enhances the energy transfer from electron plasma waves to the electron population. Although stronger magnetic fields produce a larger population of hot electrons, these electrons tend to remain confined near the quarter-critical density, where the instabilities also localize, thereby reducing the potential for hot electron transport deeper into the target. Additionally, we present a scaling analysis that quantifies hot electron generation as a function of plasma electron temperature, density scale length, and applied magnetic field strength. These findings may have important applications for controlling hot electron flux and mitigating preheat in inertial confinement fusion targets.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Planar laser-induced fluorescence system for spatiotemporal ion velocity distribution function measurements

In this work, we present a planar laser-induced fluorescence (PLIF) system for measuring two-dimensional (2D), spatiotemporally resolved ion velocity distribution functions (IVDFs). A continuous-wave tunable diode laser produces a laser sheet that irradiates the plasma, and the resulting fluorescence is captured by an intensified CCD (ICCD) camera. Fluorescence images recorded at varying laser wavelengths are converted into 2D IVDFs using the Doppler shift principle. The developed diagnostic is implemented in an electron beam generated E × B plasma with a bulk plasma density of $\sim\!\!{10^{10}}{\text{c}}{{\text{m}}^{ - 3}}$ . The developed diagnostic is validated against a conventional single-point LIF method using photomultiplier tube-based detection, while significantly reducing the total measurement time by the number of spatial positions measured. The time-resolving capability of this diagnostic is tested by oscillating the plasma between two nominal operating modes with different density profiles and triggering the ICCD camera by the externally driven plasma oscillation. The measured 2D IVDF maps reveal several signatures of ion dynamics in this plasma source, including radially outflowing ions across the electric field and anomalous ion heating at the periphery, consistent with recent kinetic simulations and theoretical studies. A possible correlation between these ion kinetic features and rotating spoke structures is discussed.

E×B plasma↗
DOE OSTI2018

Electronic spectrum and characterization of diabatic potential energy surfaces for thiophenol

The electronic spectrum of thiophenol was simulated by a normal-mode sampling approach combined with TDDFT in the Tamm–Dancoff approximation (TDA). The vertical excitation energies were compared with electronic structure calculations by completely renormalized equation-of-motion coupled cluster theory with single and double excitations and noniterative inclusion of connected triples (CR-EOM-CCSD(T)) and by multi-reference perturbation theory. The spectrum was computed both with and without solvation effects, and these spectra are compared to each other and to experiment. Using multireference-perturbation-theory adiabatic wave functions and model-space diabatization by the fourfold way, diabatic potential energy surfaces of the lowest three singlet states ( 1 ππ, 1 ππ * , and 1 n π σ * ) were constructed along the S–H stretching coordinate, the C–C–S–H torsion coordinate, and the v 16a and v 16b normal coordinates. The first two of these two are primary coordinates for the photodissociation, and the diabatic crossing seams of the three states were calculated and plotted as functions of the two coordinates. The other two coordinates are out-of-plane ring distortion modes studied to assess the extent of their role in coupling the states near the first conical intersection, and the v 16a mode was shown to be an important coupling mode there. The current study is the first step toward a detailed mechanistic analysis of the photoinduced S–H fission process of thiophenol, a test system to understand 1 n π σ * -mediated reactions, at the same time already providing a better understanding of the thiophenol electronic excitations by clarifying the assignment of the experimental results.

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

Exclusive meson photo- and electro-production, a window on the structure of hadronic matter

At high energy, exclusive meson photo- and electro-production give access to the structure of hadronic matter. At low momentum transfers, the exchange of a few Regge trajectories leads to a comprehensive account of the cross-sections. Among these trajectories, which are related to the mass spectrum of families of mesons, the Pomeron plays an interesting role as it is related to glue-ball excitations. At high momentum transfers, the exchange of these collective excitations is expected to reduce to the exchange of their simplest (quark or gluon) components. However, contributions from unitarity rescattering cuts are relevant even at high energies. In the JLab energy range, the asymptotic regime, where the players in the game are current quarks and massless gluons has not been reached yet. One has to rely on more effective degrees of freedom adapted to the scale of the probe. A consistent picture, the Partonic Non-Perturbative Regime, is emerging. The properties of its various components (dressed propagators, effective coupling constants, quark wave functions, shape of the Regge trajectories, etc) provide us with various links to hadron properties. I will review the status of the field, will put in perspective the current achievements at JLab, SLAC and Hermes, and will assess future developments that are made possible by continuous electron beams at higher energies.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Ultrafast exciton relaxation in monolayer transition metal dichalcogenides

We examine a mechanism by which excitons undergo ultrafast relaxation in common monolayer transition metal dichalcogenides. It is shown that at densities ≈1 × 10{sup 11 }cm{sup −2} and temperatures ≤60 K, excitons in well known monolayers (MoS{sub 2}, MoSe{sub 2}, WS{sub 2}, and WSe{sub 2}) exist as point-like structureless electron-hole quasi-particles. We evaluate the average rate of exciton energy relaxation due to acoustic phonons via the deformation potential and the piezoelectric coupling mechanisms and examine the effect of spreading of the excitonic wavefunction into the region perpendicular to the monolayer plane. Our results show that the exciton relaxation rate is enhanced with increase in the exciton temperature, while it is decreased with increase in the lattice temperature. Good agreements with available experimental data are obtained when the calculations are extrapolated to room temperatures. A unified approach taking into account the deformation potential and piezoelectric coupling mechanisms shows that exciton relaxation induced by phonons is as significant as defect assisted scattering and trapping of excitons by surface states in monolayer transition metal dichalcogenides.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Boron nitride on SiC(0001)

Here, in the field of van der Waals heterostructures, the twist angle between stacked two-dimensional layers has been identified to be of utmost importance for the properties of the heterostructures. In this context, we previously reported the growth of a single layer of unconventionally oriented epitaxial graphene that forms in a surfactant atmosphere [F. C. Bocquet et al., Phys. Rev. Lett. 125, 106102 (2020)]. The resulting G-R0° layer is aligned with the SiC lattice, and hence represents an important milestone towards high-quality twisted bilayer graphene, a frequently investigated model system in this field. Here, we focus on the surface structures obtained in the same surfactant atmosphere, but at lower preparation temperatures at which a boron nitride template layer forms on SiC(0001). In a comprehensive study based on complementary experimental and theoretical techniques, we find—in contrast to the literature—that this template layer is a hexagonal B x N y layer, but not high-quality hBN. It is aligned with the SiC lattice and gradually replaced by low-quality graphene in the 0° orientation of the B x N y template layer upon annealing.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Diffuse scattering from correlated electron systems

The role of inhomegeneity in determining the properties of correlated electron systems is poorly understood because of the dearth of structural probes of disorder at the nanoscale. Advances in both neutron and x-ray scattering instrumentation now allow comprehensive measurements of diffuse scattering in single crystals over large volumes of reciprocal space, enabling structural correlations to be characterized over a range of length scales from 5 to 200 angstroms or more. When combined with new analysis tools, such as three-dimensional difference pair-distribution functions, these advanced capabilities have produced fresh insights into the interplay of structural fluctuations and electronic properties in a broad range of correlated electron materials. This review describes recent investigations that have demonstrated the importance of understanding structural inhomogeneity pertaining to phenomena as diverse as superconductivity, charge density wave modulations, metal-insulator transitions, and multipolar interactions.

36 MATERIALS SCIENCE↗