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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 1,243 records · Page 69
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Socorro Electronic Structure Software

Socorro can be used to compute the ground-state electron density for a periodically repeated simulation cell in which the external potential is obtained from norm-conserving pseudopotentials or projector-augmented-wave functions. The ground-state electron density is computed by summation over one-electron orbitals which are obtained using the Kohn-Sham formulation of density-functional theory and which are expanded in a plane-wave basis. Various quantities can be computed from the ground-state solution, including atomic forces which can be used to optimize atom positions in the simulation cell and to perform molecular dynamics simulations.

Foiles, Stephen M↗
DOE OSTI2018

Electronic and structural response to pressure in the hyperkagome-lattice Na 3 Ir 3 O 8

Here, the hyper-kagome lattice iridate Na 3 Ir 3 O 8 , closely related to spin liquid candidate Na 4 Ir 3 O 8 , is unusual in that spin-orbit interactions acting on the 1/3-filled J eff = 1/2 state lead to a semimetallic ground state, in contrast to the conventional insulating Mott state stabilized by S-O interactions in the 1/2-filled J eff = 1/2 state of other iridates including Na 4 Ir 3 O 8 . We have studied the evolution of crystal structure, electronic structure, and transport in Na 3 Ir 3 O 8 under high pressure using x-ray diffraction, x-ray absorption near edge structure, and electrical resistance measurements in a diamond anvil cell. The study was augmented by the use of ab initio calculations, which provided insight into pressure-induced changes in crystal and electronic structure. We found that Na 3 Ir 3 O 8 transforms from a semimetal to an insulator under pressure, with an estimated energy gap that increases to about 130 meV at P similar to 9 GPa. At approximately 10 GPa, a cubic-to-monoclinic structural transition takes place between two insulating phases. This structural transition features a sizable volume collapse and a high-pressure phase characterized by apparent dimerization of Ir-Ir distances, wide dispersion of Ir-O-Ir bond angles, and an increase in the occupation of 5 d states. Although the energy gap is reduced in the high-pressure phase, insulating behavior remains to the highest pressures similar to 1 Mbar. The strongly pressure-dependent insulating gap shows a positive correlation with the expectation value of the angular part of the S-O interaction, < L • S >, which may indicate an active role of S-O interactions in stabilizing the insulating state that emerges in the compressed Na 3 Ir 3 O 8 structure.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Vibrational spectra and electronic structure of 11-vertex boron-containing clusters: a comparative study of [B{sub 11}H{sub 11}]{sup 2–}, [CB{sub 10}H{sub 11}]{sup –}, and C{sub 2}B{sub 9}H{sub 11}

Vibrational spectroscopy studies of 11-vertex boron-containing clusters [B{sub 11}H{sub 11}]{sup 2–}(1), [2-CB{sub 10}H{sub 11}]{sup –} (2), and 2,3-C{sub 2}B{sub 9}H{sub 11} (3) revealed two low-frequency large-amplitude modes in their spectra and, therefore, structural nonrigidity of these polyhedra in contrast to related 12-, 10-, and 6-vertex closo-clusters. The nonrigidity originates from specific features of the electron density distribution. According to calculations within the framework of the 'Atoms in Molecule' (AIM) theory, these polyhedra are characterized by the lack of many bond paths localized on corresponding edges, in particular, between boron atoms with coordination numbers of 6 and 5 (6k and 5k). Consequently, these polyhedra are composed of not only trigonal faces, i.e., formally do not have the closo-structure that was traditionally ascribed to them based on formal count of (2n + 2) valence electrons. According to calculations of three-center delocalization indices, the absence of bond paths is not equivalent to the lack of interaction between corresponding atoms since this interaction occurs through open three-center bonds. The mechanism and reasons for signal averaging observed in {sup 11}B NMR spectra of compounds 1 and 2 in contrast to 3 are analyzed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

On the connection between microbursts and nonlinear electronic structures in planetary radiation belts

Using a dynamical-system approach, we have investigated the efficiency of large-amplitude whistler waves for causing microburst precipitation in planetary radiation belts by modeling the microburst energy and particle fluxes produced as a result of nonlinear wave–particle interactions. We show that wave parameters, consistent with large-amplitude oblique whistlers, can commonly generate microbursts of electrons with hundreds of keV-energies as a result of Landau trapping. Relativistic microbursts (>1 MeV) can also be generated by a similar mechanism, but require waves with large propagation angles θ{sub kB}>50{sup ∘} and phase-speeds v{sub Φ}⩾c/9. Using our result for precipitating density and energy fluxes, we argue that holes in the distribution function of electrons near the magnetic mirror point can result in the generation of double layers and electron solitary holes consistent in scales (of the order of Debye lengths) to nonlinear structures observed in the radiation belts by the Van Allen Probes. Our results indicate a relationship between nonlinear electrostatic and electromagnetic structures in the dynamics of planetary radiation belts and their role in the cyclical production of energetic electrons (E⩾100 keV) on kinetic timescales, which is much faster than previously inferred.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

Electronic structure of nitrogen-doped lutetium hydrides

First-principles density functional theory (DFT) calculations of supercell structures based on N-doped Fm $\bar3$m LuH 3 reveal configurations of Fm $\bar3$m Lu 8 H 23–x N that exhibit novel electronic properties such as flat bands, sharply peaked densities of states (van Hove singularities, vHs), and intersecting Dirac cones near the Fermi energy (E F ). These electronic properties are present when N substitutes H in the octahedral interstices of Fm $\bar3$ m LuH 3 . These structures also exhibit an interconnected metallic hydrogen network, a common feature of high-T c hydride superconductors. Electronic property systematics gives an estimate of T c for one structure that is well above the critical temperatures predicted for structures considered previously. DFT + U has an especially strong effect on one of the structures considered, enhancing the vHs and flat bands near E F . Finally, these results provide a basis for understanding the electronic properties observed for nitrogen-doped lutetium hydride.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Synthesis, Structural, Electronic, and Magnetic Properties of Cubic Perovskite La{sub 1−x}Ba{sub x}MnO{sub 3} (0.125 ≤ x ≤ 0.875) for Spintronic Devices

In this study, La{sub 0.5}Ba{sub 0.5}MnO{sub 3} has been synthesized by hydrothermal method. Crystal structure and morphology are determined by x-ray diffraction and scanning electron microscopy. It is observed that Ba-doped LaMnO{sub 3} (LMO) has the same cubic crystal structure as the host material with space group Pm3̄m. Half of the La atoms are replaced by Ba in the composition. Further, the electronic and magnetic structures are investigated by solving the Kohn-Sham equation with the full-potential linearized augmented plane wave method (FP-LAPW), with GGA+U approximation for exchange and correlation, for Ba concentration from 12.5 to 87.5%. The system is half-metallic ferromagnetic (FM) up to 55% and then converts into anti-ferromagnetic (AFM). This happens due to the onset of super exchange on increasing Ba concentrations. It is suggested that Ba-doped LMO is the best material for the fabrication of an exchange-biased spin valve. The spacer material can be any non-magnetic cubic perovskite such as BaTiO{sub 3} while the FM and AFM layers can be made of Ba-doped LMO with different concentrations of Ba. .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Electronic Structure and Ferromagnetism in Zincblende Zn{sub 1−x}Co{sub x}S Nanoparticles

We have prepared Zn{sub 1−x}Co{sub x}S nanoparticles (NPs) and studied their local-geometric, electronic, and magnetic properties. X-ray diffraction analyses have indicated that NPs with average crystallite sizes of 2.2 ∼ 2.9 nm are single phase and crystallize in the zincblende-type structure. Cobalt ions with oxidation state + 2 (Co{sup 2+}) replaced for Zn{sup 2+} and almost unchanged the zincblende-type structure of the ZnS host lattice. Interestingly, all samples show room-temperature ferromagnetism and ferromagnetic order increases with increasing Co content (x) in Zn{sub 1−x}Co{sub x}S NPs. With the results obtained from analyzing the local-geometric structures at Zn and Co K-edges and photoluminescence spectra, we believe that ferromagnetism in Zn{sub 1−x}Co{sub x}S NPs is related to intrinsic defects and exchange interactions between Co{sup 2+} ions. We have also reviewed the recent studies on ZnS-based dilute-magnetic materials.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2017

Electronic Structure and Band Alignment at the NiO and SrTiO 3 p–n Heterojunctions

Understanding the energetics at the interface including the alignment of valence and conduction bands, built-in potentials, and ionic and electronic reconstructions, is an important challenge in designing oxide interfaces that have controllable multi-functionalities for novel (opto-)electronic devices. In this work, we report detailed investigations on the hetero-interface of wide bandgap p-type NiO and n-type SrTiO3 (STO). We show that despite a large lattice mismatch (~7%) and dissimilar crystal structure, high-quality NiO and Li doped NiO (LNO) thin films can be epitaxially grown on STO(001) substrates through a domain matching epitaxy (DME) mechanism. X-ray photoelectron spectroscopy (XPS) studies indicate that NiO/STO heterojunctions form a type II “staggered” band alignment. In addition, a large built-in potential of up to 0.97 eV was observed at the interface of LNO and Nb doped STO (NbSTO). The LNO/NbSTO p-n heterojunctions exhibit a large rectification ratio of 2×103, but also a large ideality factor of 4.3. The NiO/STO p-n heterojunctions have important implication for applications in photocatalysis and photodetector as the interface provides favourable energetics for facile separation and transport of photogenerated electrons and holes.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Optically induced lattice deformations, electronic structure changes, and enhanced superconductivity in YBa 2 Cu 3 O 6.48

Resonant optical excitation of apical oxygen vibrational modes in the normal state of underdoped YBa 2 Cu 3 O 6+x induces a transient state with optical properties similar to those of the equilibrium superconducting state. Amongst these, a divergent imaginary conductivity and a plasma edge are transiently observed in the photo-stimulated state. Femtosecond hard x-ray diffraction experiments have been used in the past to identify the transient crystal structure in this non-equilibrium state. Here, we start from these crystallographic features and theoretically predict the corresponding electronic rearrangements that accompany these structural deformations. Using density functional theory, we predict enhanced hole-doping of the CuO 2 planes. The empty chain Cu dy 2 -z 2 orbital is calculated to strongly reduce in energy, which would increase c-axis transport and potentially enhance the interlayer Josephson coupling as observed in the THz-frequency response. From these results, we calculate changes in the soft x-ray absorption spectra at the Cu L -edge. As a result, femtosecond x-ray pulses from a free electron laser are used to probe changes in absorption at two photon energies along this spectrum and provide data consistent with these predictions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Impact of n -Butylammonium Bromide on the Chemical and Electronic Structure of Double-Cation Perovskite Thin Films

2D/3D perovskite heterostructures have emerged as a promising material composition to reduce nonradiative recombination in perovskite-based LEDs and solar cells. Such heterostructures can be created by a surface treatment with large organic cations, for example, n-butylammonium bromide (BABr). To understand the impact of the BABr surface treatment on the double-cation (Cs 0.17 FA 0.83 Pb(I 0.6 Br 0.4 ) 3 ) (FA = formamidinium) perovskite thin film and further optimize the corresponding structures, an in-depth understanding of the chemical and electronic properties of the involved surfaces, interfaces, and bulk is required. We study the impact of the BABr treatment with a combination of surface-sensitive X-ray photoelectron spectroscopy and bulk-sensitive resonant inelastic soft X-ray scattering (RIXS). A quantitative analysis of the BABr-treated perovskite thin film shows a modified chemical perovskite surface environment of carbon, nitrogen, bromine, iodine, and lead, indicating that the treatment leads to a perovskite surface with a modified composition and bonding structure. With K-edge RIXS, the local environment at the nitrogen and carbon atoms is probed, allowing us to identify the presence of BABr in the perovskite bulk albeit with a modified bonding environment. This, in turn, identifies a "hidden parameter" for the optimization of the BABr treatment and overall performance of 2D/3D perovskite solar cell absorbers.

2D/3D perovskite heterostructure↗
DOE OSTI2014

Electronic structure of ordered double perovskite Ba{sub 2}CoWO{sub 6}

Ba{sub 2}CoWO{sub 6} (BCoW) has been synthesized in polycrystalline form by solid state reaction at 1200 °C. Structural characterization of the compound was done through X-ray diffraction (XRD) followed by Rietveld analysis of the XRD pattern. The crystal structure is cubic, space group Fm-3m (No. 225) with the lattice parameter, a = 8.210. Optical band-gap of the present system has been calculated using the UV-Vis Spectroscopy and Kubelka-Munk function, it’s value being 2.45 eV. A detailed study of the electronic properties has also been carried out using the density functional theory (DFT) techniques implemented on WIEN2k. Importance of electron-electron interaction between the Co ions leading to half-metallic behavior, crystal and exchange splitting together with the hybridization between O and Co, W has been investigated using the total and partial density of states.

36 MATERIALS SCIENCE↗
DOE OSTI2025

An Ab Initio Electronic Structure Investigation of the Ground and Excited States of ScH + , YH + , and LaH +

Multireference configuration interaction (MRCI), Davidson-corrected MRCI (MRCI+Q), coupled-cluster singles, doubles, and perturbative triples [CCSD(T)], and frozen-core full configuration interaction (fcFCI) calculations were carried out using large, correlation-consistent basis sets to investigate the excited states of the Sc atom and the spin–free and spin–orbit coupled potential energy profiles, energetics, spectroscopic constants, and electron populations of low-lying states of MH + (M = Sc, Y, La). The core electron correlation effects, complete basis set effects, and spin–orbit coupling effects were also evaluated. The first four electronic states of all MH + are 1 2 Δ, 1 2 Σ + , 1 2 Π, and 2 2 Σ + with 1σ 2 1δ 1 , 1σ 2 2σ 1 , 1σ 2 1π 1 , and 1σ 2 3σ 1 single-reference electron configurations, respectively. These states of MH + can be represented by the M 2+ H – ionic structure. The ground states of ScH + , YH + , and LaH + are 1 2 Δ 3/2 , 1 2 Σ + 1/2 , and 1 2 Δ 3/2 with 55.45, 60.54, and 62.34 kcal/mol bond energies, respectively. The core electron correlation was found to be vital for gaining accurate predictions on the ground and excited state properties of MH + . The spin–orbit coupling effects are minor for ScH + but become substantial moving to YH + and LaH + . Overall, the results of this work are in good agreement with the limited set of experimental findings of MH + available in the literature and will be of use for future investigations. Furthermore, the theoretical approaches, findings, and trends reported here are expected to aid studies of similar species.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

Effect of electron correlation on the electronic structure and spin-lattice coupling of high- T c cuprates: Quantum Monte Carlo calculations

Electron correlation effects are particularly strong in high-temperature superconducting materials. Devising an accurate description of these materials has long been a challenge, with these strong correlation effects historically being considered impossible or impractical to simulate computationally. Using quantum Monte Carlo techniques, we have explicitly simulated electron correlations in several cuprate materials from first principles. These simulations accurately reproduce many important physical quantities of these materials, including the interaction-induced gap and superexchange coupling between copper spins, with no additional parameters beyond fundamental constants. We further investigate the dimensionless spin-lattice coupling parameter in the parent materials, showing that it varies dramatically, between 0.1 and 1.0, depending on the interlayer. Furthermore, this result indicates that the lattice and magnetic degrees of freedom are not independent in these systems, which may have ramifications for the origin of superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Novel Relativistic Electronic Structure Theories for Actinide-Containing Compounds

Actinides of importance to basic energy sciences contain electrons moving at speed comparable to the speed of light. Reliable computational simulation of these electrons and hence actinide chemistry requires accurate description of relativistic effects. The present project advances computational actinide chemistry with development of new methodologies, algorithms, and computer programs in relativistic quantum chemistry, as well as applications to actinide chemistry and spectroscopy. A new “electrons-only” exact two-component approach has been developed to provide efficient treatments of relativistic effects, while maintaining chemical accuracy. New computational algorithms developed here extend the applicability of relativistic electron-correlation methods to larger molecules. The method-development work in this project also features the first implementation of analytic gradient technique for relativistic electron-correlation methods, which provides significantly enhanced ability to compute properties for molecules containing actinides. The applicability and usefulness of these new methods and computer programs have been demonstrated in calculations of actinide-containing molecules to facilitate understanding of actinide chemistry and spectroscopy.

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

Tuning the Geometric and Electronic Structure of Synthetic High-Valent Heme Iron(IV)-Oxo Models in the Presence of a Lewis Acid and Various Axial Ligands

High-valent ferryl species (e.g., (Por)Fe IV =O, Cmpd-II) are observed or proposed key oxidizing intermediates in the catalytic cycles of heme-containing enzymes (P-450s, peroxidases, catalases, and cytochrome c oxidase) involved in biological respiration and oxidative metabolism. Herein, various axially ligated iron(IV)-oxo complexes were prepared to examine the influence of the identity of the base. These were generated by addition of various axial ligands (1,5-dicyclohexylimidazole (DCHIm), a tethered-imidazole system, and sodium derivatives of 3,5-dimethoxyphenolate and imidazolate). Characterization was carried out via UV–vis, electron paramagnetic resonance (EPR), 57 Fe Mössbauer, Fe X-ray absorption (XAS), and 54/57 Fe resonance Raman (rR) spectroscopies to confirm their formation and compare the axial ligand perturbation on the electronic and geometric structures of these heme iron(IV)-oxo species. Mössbauer studies confirmed that the axially ligated derivatives were iron(IV) and six-coordinate complexes. XAS and 54/57 Fe rR data correlated with slight elongation of the iron-oxo bond with increasing donation from the axial ligands. The first reported synthetic H-bonded iron(IV)-oxo heme systems were made in the presence of the protic Lewis acid, 2,6-lutidinium triflate (LutH + ), with (or without) DCHIm. Mössbauer, rR, and XAS spectroscopic data indicated the formation of molecular Lewis acid ferryl adducts (rather than full protonation). Here, the reduction potentials of these novel Lewis acid adducts were bracketed through addition of outer-sphere reductants. The oxidizing capabilities of the ferryl species with or without Lewis acid vary drastically; addition of LutH + to F 8 Cmpd-II (F 8 = tetrakis(2,6-difluorophenyl)porphyrinate) increased its reduction potential by more than 890 mV, experimentally confirming that H-bonding interactions can increase the reactivity of ferryl species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Structural and electronic properties of polar MnO ultrathin film grown on Ag(111)

Surface electronic structure of ultrathin polar MnO film was studied by Low-energy Electron Diffraction (LEED) and Photoemission Spectroscopic (PES) techniques. Epitaxial monolayer to facet formation with increasing film thickness has been observed by LEED. Our LEED result shows p(2x2) surface reconstruction along with facet formation, stabilize the polar MnO(111) surface. The core levels and the valence band electronic structure of MnO films have been studied as a function of film thickness using X-ray and ultraviolet photoelectron spectroscopy techniques.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Model of Electronic Structure and Superconductivity in Orbitally Ordered FeSe

We provide a band structure with low-energy properties consistent with recent photoemission and quantum oscillation measurements on FeSe, assuming mean-field-like site- and/or bond-centered ferro-orbital ordering at the structural transition. Here, we show how the resulting model provides a consistent explanation of the temperature dependence of the measured Knight shift and the spin-relaxation rate. Furthermore, the superconducting gap structure obtained from spin-fluctuation theory exhibits nodes on the electron pockets, consistent with the V-shaped density of states obtained by tunneling spectroscopy on this material, and the temperature dependence of the London penetration depth.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗