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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 901 records · Page 50
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Ab initio calculations of exciton effects in optical spectra of an α-B{sub 12} crystal

The dielectric functions and energy loss spectrum of electrons of a rhombohedral α-B{sub 12} crystal are studied both in the single-particle and many-particle approximations using Bethe–Salpeter equations. The opposite roles of different contributions to exciton effects are discussed. The anisotropy of dielectric functions is shown, which demonstrates their high sensitivity with respect to the three-dimensional packing of icosahedrons. The influence of the coherent mixing of electronic and exciton states on the redistribution of oscillator strengths is found. The position of the plasmon of valence electrons and the high-frequency permittivity are found to be consistent with experimental data. The correlation between the distribution of oscillator strengths and features of the density of electronic states is discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Ab initio leading order effective potential for elastic proton scattering based on the symmetry-adapted no-core shell model

Calculating microscopic optical potentials for elastic scattering at intermediate energies from light nuclei in an ab initio fashion within the Watson expansion has been established within the last few years. Based on the Watson expansion of the multiple scattering series, we employ a nonlocal translationally invariant nuclear density derived within the symmetry-adapted no-core shell model (SA-NCSM) framework from a chiral next-to-next-to-leading order (NNLO) nucleon-nucleon interaction and the very same interaction for a consistent full-folding calculation of the effective (optical) potential for nucleon-nucleus scattering for medium-heavy nuclei. The leading order effective (optical) folding potential is computed by integrating over a translationally invariant SA-NCSM one-body scalar density, spin-projected momentum distribution, and the Wolfenstein amplitudes 𝐴, 𝐶, and 𝑀. The resulting nonlocal potentials serve as input for a momentum space Lippmann-Schwinger equation. In the SA-NCSM, the model space is systematically up-selected using Sp⁡(3,ℝ) symmetry considerations. For the light nucleus of 6 He, we establish a systematic selection scheme in the SA-NCSM for scattering observables. Then, we apply this scheme to calculations of scattering observables, such as differential cross sections, analyzing powers, and spin rotation functions for elastic proton scattering from 20 Ne and 40 Ca in the energy regime between 65 and 200 MeV, and compare to available data. Furthermore, our calculations show that the leading order effective nucleon-nucleus potential in the Watson expansion of multiple scattering theory obtained from an up-selected SA-NCSM model space describes 40 Ca elastic scattering observables reasonably well to about 60 degrees in the center-of-mass frame, which coincides roughly with the validity of the NNLO chiral interaction used to calculate both the nucleon-nucleon amplitudes and the one-body scalar and spin nuclear densities.

Ab initio calculations↗
DOE OSTI2018

Molecular Dynamics Modeling of the Structure and Na + -Ion Transport in Na 2 S + SiS 2 Glassy Electrolytes

Solid-state sodium batteries, a relatively safe and potentially cost-effective energy-storage technology, have attracted increasing scientific attention recently for application in stationary grid-scale energy storage. Identifying solid electrolytes with high electrochemical stability and high Na+-ion conductivity at room temperature is critically important to enable high energy densities with enhanced rate capabilities. We evaluated sodium sulfide silicon sulfide, xNa 2 S + (1 - x)SiS 2 , glasses as potential glassy solid electrolytes (GSEs) using molecular dynamics (MD) simulations. We employed ab initio MD to determine ion conduction mechanisms, to calculate energy barriers for ion hops, and to correlate these to the local short-range structure of 0.50Na 2 S + 0.50SiS 2 glass. To simulate much larger systems for accurately calculating the ionic conductivity, we parameterized empirical Buckingham-type potential and performed classical MD simulations. After validating these calculations by comparing the structure obtained from MD to that from X-ray scattering data, we calculated the ionic conductivity of these glasses for the range of 0.33 ≤ x ≤ 0.67 compositions. The calculated ionic conductivities at room temperature were in the range of similar to 10 -5 S/cm for the x = 0.50 composition and increased significantly with sodium sulfide (x) content. Furthermore, these calculations provide theoretical insights into the role of Na 2 S content on the ionic conductivity of GSEs aiding in the selection of specific compositions to enhance the ionic conductivity.

25 ENERGY STORAGE↗
DOE OSTI2022

Multi-task graph neural networks for simultaneous prediction of global and atomic properties in ferromagnetic systems *

Abstract We introduce a multi-tasking graph convolutional neural network, HydraGNN, to simultaneously predict both global and atomic physical properties and demonstrate with ferromagnetic materials. We train HydraGNN on an open-source ab initio density functional theory (DFT) dataset for iron-platinum with a fixed body centered tetragonal lattice structure and fixed volume to simultaneously predict the mixing enthalpy (a global feature of the system), the atomic charge transfer, and the atomic magnetic moment across configurations that span the entire compositional range. By taking advantage of underlying physical correlations between material properties, multi-task learning (MTL) with HydraGNN provides effective training even with modest amounts of data. Moreover, this is achieved with just one architecture instead of three, as required by single-task learning (STL). The first convolutional layers of the HydraGNN architecture are shared by all learning tasks and extract features common to all material properties. The following layers discriminate the features of the different properties, the results of which are fed to the separate heads of the final layer to produce predictions. Numerical results show that HydraGNN effectively captures the relation between the configurational entropy and the material properties over the entire compositional range. Overall, the accuracy of simultaneous MTL predictions is comparable to the accuracy of the STL predictions. In addition, the computational cost of training HydraGNN for MTL is much lower than the original DFT calculations and also lower than training separate STL models for each property.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Glass-like energy and property landscape of Pt nanoclusters

Pt nanoclusters play an important role in catalysis-related applications. Essential to their activities are their geometries and energy landscapes. In this work, we studied the energy landscapes of Pt clusters using a parallel differential evolution optimization algorithm and an accelerated ab initio atomic relaxation method, which allowed us to explore unprecedentedly large numbers of geometry local minima at ab initio level. We found many lower-energy isomers with low symmetry in their geometry. The energy landscapes were demonstrated to be glass-like with a large number of local minimum structures close to the global minimum. The electronic and magnetic properties of most glass-like local minima were dramatically different from the global minimum, and they should be observed in the experimental measurements. The connections between these local minima were further analyzed using data mining techniques.

Chen, Zhanghui↗
DOE OSTI2017

Construction of ground-state preserving sparse lattice models for predictive materials simulations

First-principles based cluster expansion models are the dominant approach in ab initio thermodynamics of crystalline mixtures enabling the prediction of phase diagrams and novel ground states. However, despite recent advances, the construction of accurate models still requires a careful and time-consuming manual parameter tuning process for ground-state preservation, since this property is not guaranteed by default. In this paper, we present a systematic and mathematically sound method to obtain cluster expansion models that are guaranteed to preserve the ground states of their reference data. The method builds on the recently introduced compressive sensing paradigm for cluster expansion and employs quadratic programming to impose constraints on the model parameters. The robustness of our methodology is illustrated for two lithium transition metal oxides with relevance for Li-ion battery cathodes, i.e., Li 2x Fe 2(1-x) O 2 and Li 2x Ti 2(1-x) O 2 , for which the construction of cluster expansion models with compressive sensing alone has proven to be challenging. We demonstrate that our method not only guarantees ground-state preservation on the set of reference structures used for the model construction, but also show that out-of-sample ground-state preservation up to relatively large supercell size is achievable through a rapidly converging iterative refinement. This method provides a general tool for building robust, compressed and constrained physical models with predictive power.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Palladium at high pressure and high temperature: A combined experimental and theoretical study

Palladium is one of the most important technological materials, yet its phase diagram remains poorly understood. At ambient conditions, its solid phase is face-centered cubic (fcc). However, another solid phase of Pd, body-centered cubic (bcc), was very recently predicted in two independent theoretical studies to occur at high pressures and temperatures. In this work, we report an experimental study on the room-temperature equation of state (EOS) of Pd to a pressure of 80 GPa, as well as a theoretical study on the phase diagram of Pd including both fcc-Pd and bcc-Pd. Our theoretical approach consists in ab initio quantum molecular dynamics (QMD) simulations based on the Z methodology which combines both direct Z method for the simulation of melting curves and inverse Z method for the calculation of solid–solid phase transition boundaries. We obtain the melting curves of both fcc-Pd and bcc-Pd and an equation for the fcc–bcc solid–solid phase transition boundary as well as the thermal EOS of Pd which is in agreement with experimental data and QMD simulations. We uncover the presence of another solid phase of Pd on its phase diagram, namely, random hexagonal close-packed (rhcp), and estimate the location of the rhcp-bcc solid–solid phase transition boundary and the rhcp–fcc–bcc triple point. We also discuss the topological similarity of the phase diagrams of palladium and silver, the neighbor of Pd in the periodic table. We argue that Pd is a reliable standard for shock-compression studies and present the analytic model of its principal Hugoniot in a wide pressure range.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ab Initio Calculation of the Alpha-Particle Monopole Transition Form Factor

Here we present a parameter-free ab initio calculation of the α-particle monopole transition form factor in the framework of nuclear lattice effective field theory. We use a minimal nuclear interaction that was previously used to reproduce the ground state properties of light nuclei, medium-mass nuclei, and neutron matter simultaneously with no more than a few percent error in the energies and charge radii. The results for the monopole transition form factor are in good agreement with recent precision data from Mainz.

4He↗
DOE OSTI2024

Palladium at high pressure and high temperature: A combined experimental and theoretical study

Palladium is one of the most important technological materials, yet its phase diagram remains poorly understood. At ambient conditions, its solid phase is face-centered cubic (fcc). However, another solid phase of Pd, body-centered cubic (bcc), was very recently predicted in two independent theoretical studies to occur at high pressures and temperatures. In this work, we report an experimental study on the room-temperature equation of state (EOS) of Pd to a pressure of 80 GPa, as well as a theoretical study on the phase diagram of Pd including both fcc-Pd and bcc-Pd. Our theoretical approach consists in ab initio quantum molecular dynamics (QMD) simulations based on the Z methodology which combines both direct Z method for the simulation of melting curves and inverse Z method for the calculation of solid–solid phase transition boundaries. We obtain the melting curves of both fcc-Pd and bcc-Pd and an equation for the fcc–bcc solid– solid phase transition boundary as well as the thermal EOS of Pd which is in agreement with experimental data and QMD simulations. We uncover the presence of another solid phase of Pd on its phase diagram, namely, random hexagonal close-packed (rhcp), and estimate the location of the rhcp-bcc solid–solid phase transition boundary and the rhcp–fcc–bcc triple point. We also discuss the topological similarity of the phase diagrams of palladium and silver, the neighbor of Pd in the periodic table. We argue that Pd is a reliable standard for shock-compression studies and present the analytic model of its principal Hugoniot in a wide pressure range.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Revealing the strength of three-nucleon interactions with the proposed Einstein Telescope

Nuclear systems, ranging from atomic nuclei to dense matter probed in neutron stars, are governed by strong interactions. Three-nucleon forces have been found to be a crucial ingredient for the reliable description of these systems. Here, in this work, we explore how astrophysical data on neutron stars and their mergers from current and next-generation observatories will enable us to distinguish nuclear Hamiltonians. In particular, we investigate two different nuclear Hamiltonians that have been adjusted to reproduce two-nucleon scattering data and properties of light nuclei, but differ in the three-nucleon interactions among neutrons. We find that no significant constraints can be obtained from current data, but that the proposed Einstein Telescope could provide strong evidence to distinguish among these Hamiltonians.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2016

Combining state-of-the-art experiment and ab initio calculations for a better understanding of the interplay between valence, magnetism and structure in Eu compounds at high pressure

Here, we describe how first principle calculations can play a key role in the interpretation of X-ray absorption near-edge structure (XANES) and X-ray magnetic circular dichroism (XMCD) spectra for a better understanding of emergent phenomena in condensed matter physics at high applied pressure. Eu compounds are used as case study to illustrate the advantages of this methodology, ranging from studies of electronic charge transfer probed by quadrupolar and dipolar contributions, to accurately determining electronic valence, and to inform about the influence of pressure on RKKY interactions and magnetism. This description should help advance studies where the pressure dependence of XANES and XMCD data must be tackled with the support of theoretical calculations for a proper understanding of the electronic properties of materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

ROVIBRATIONAL LINE LISTS FOR NINE ISOTOPOLOGUES OF THE CO MOLECULE IN THE X {sup 1}Σ{sup +} GROUND ELECTRONIC STATE

Extensive rovibrational line lists were computed for nine isotopologues of the CO molecule, namely, {sup 12}C{sup 16}O, {sup 12}C{sup 17}O, {sup 12}C{sup 18}O, {sup 13}C{sup 16}O, {sup 13}C{sup 17}O, {sup 13}C{sup 18}O, {sup 14}C{sup 16}O, {sup 14}C{sup 17}O, and {sup 14}C{sup 18}O in the ground electronic state with v ≤ 41, Δv ≤ 11, and J ≤ 150. The line intensity and position calculations were carried out using a newly determined piece-wise dipole moment function (DMF) in conjunction with the wavefunctions calculated from an experimentally determined potential energy function from Coxon and Hajigeorgiou. A direct-fit method that simultaneously fits all the reliable experimental rovibrational matrix elements has been used to construct the dipole moment function near equilibrium internuclear distance. In order to extend the amount and quality of input experimental parameters, new Cavity Ring Down Spectroscopy experiments were carried out to enable measurements of the lines in the 4-0 band with low uncertainty as well as the first measurements of lines in the 6-0 band. A new high-level ab initio DMF, derived from a finite field approach has been calculated to cover internuclear distances far from equilibrium. Accurate partition sums have been derived for temperatures up to 9000 K. In addition to air- and self-induced broadening and shift parameters, those induced by CO{sub 2} and H{sub 2} are now provided for planetary applications. A complete set of broadening and shift parameters was calculated based on sophisticated extrapolation of high-quality measured data. The line lists, which follow HITRAN formalism, are provided as supplementary material.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Calculations of electronic excitation by protons and alpha particles in silicon

This paper presents an ab initio method of calculating the valence electron contribution to the stopping and interaction cross sections of swift ions in matter using linear response calculations of the dielectric function in crystals. We estimate the contribution to the stopping and cross sections by repeated electron capture and stripping of the projectile ion by the medium. We also predict the electronic stopping of protons and alpha particles in silicon and compare to measured values. The predictions generally agree with the data at ion speeds greater than 1 atomic unit. We find that electron capture and stripping is at most a small contribution to the stopping for both ions studied.

electron excitation, silicon, nuclear interactions↗
DOE OSTI2019

Analysis of Methods of Investigation of the Vibration–Rotation Spectrum of Monomers and Dimers of Sulphur Hexafluoride Isotopes

The stability of the system of sulphur hexafluoride dimer SF{sub 6} under the action of external laser radiation has been estimated using ab initio quantum-chemical calculations of the vibration–rotation spectrum of SF{sub 6} monomers as well as homo- and heterodimers. It is noted that for simple CO molecule as an example, the most widely used method of calculations based on the Hessian matrix approach cannot serve as a reliable instrument in quantitative calculations of some molecular systems. As a potential analog, we have tested the algorithm for obtaining the vibration–rotation spectrum based on molecular dynamics data.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1984

A measurement of the vibrational band strength for the v3 band of the HO2 radical

Laboratory measurements of the v(3) band strength of HO2 using a tunable diode laser to measure the absorption strength of a vibration-rotation line in the P branch near 1080/cm are reported. The HO2 is generated in a discharge-flow system by reaction of fluorine atoms with excess H2O2: F + H2O2 - HO2 + HF. The HO2 concentration is determined from measurements of F-atom concentrations using both chemical titration with Cl2 and tunable diode laser absorption by the F-atom spin-orbit transition near 404/cm. The experimental data are consistent with a value of k(3) = (1.6 + or - 0.3) x 10 to the 12th cu cm/s and a ratio k(4)/k(1) = 1.0 + or - 0.4. The line strength for the 6(15) - 7(16)F(1) transition is 2.9 x 10 to the -21 sq cm/molecule/cm, which corresponds to a v(3) band strength of 35 + or - 9/sq cm/(STP atm). This value is a factor of 1.6 to 6 lower than previous ab initio calculations.

Zahniser, M. S.↗
NASA NTRS1992

An extensive ab initio study of the structures, vibrational spectra, quadratic force fields, and relative energetics of three isomers of Cl2O2

Quantum mechanical computational methods are employed for an ab initio investigation of: (1) the molecular properties of the lowest isomers of the ClO dimer; and (2) predicted molecular and thermochemical properties. Techniques employed include electron correlation and particularly singles and doubles coupled-cluster (CCSD) theory with or without perturbational estimates of the effects of connected triple excitations. The isomers ClOClO and ClClO2 are found to have higher energies than the ClOOCl isomer, and the theoretical vibrational frequencies of the isomers are well correlated with experimental data. Experimental values of the heat of formation for the isomers are also compared with calculations based on an isodesmic reaction with Cl2O, H2O, and HOOH.

Lee, Timothy J.↗