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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 505 records · Page 28
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Electronic structure and magnetism in g-C{sub 4}N{sub 3} controlled by strain engineering

Regulation of magnetism and half-metallicity has attracted much attention because of its potential in spintronics. The magnetic properties and electronic structure of graphitic carbon nitride (g-C{sub 4}N{sub 3}) with external strain are determined theoretically based on the density function theory and many-body perturbation theory (G{sub 0}W{sub 0}). Asymmetric deformation induced by uniaxial strain not only regulates the magnetic characteristics but also leads to a transformation from half-metallicity to metallicity. However, this transition cannot occur in the structure with symmetric deformation induced by biaxial strain. Our results suggest the use of strain engineering in metal-free spintronics applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Pressure dependence of half metallic behavior of Co{sub 2}VZ (Z=Si, Ge)-An ab initio Study

The structural, electronic and magnetic properties of Co-based Heusler compounds Co{sub 2}VZ (Z=Si, Ge) under pressure are studied using first-principles density functional theory. The total magnetic moment decreases on compression. Under application of external pressure, the valence band and conduction band are shifted downward which leads to modification of electronic structure. True half metallic to nearly half metallic transition is observed at 30 GPa, 50 GPa for Co{sub 2}VSi and Co{sub 2}VGe respectively. Around 100 GPa, Co{sub 2}VGe shows complete metallic behavior. The half metal to metal transition is accompanied by quenching of magnetic moment.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Atomic and electron structure of reconstructed (111) surface in ZnSe and CdSe crystals

The atomic and electron structure of four variants of polar (111)-(2 × 2) surfaces in ZnSe and CdSe terminated by a cation, namely, the ideal, relaxed, reconstructed, and relaxed after reconstruction surfaces, are calculated for the first time from the first principles. The surface is simulated by a film with a thickness of 12 atomic layers and a vacuum gap of ~16 Å in the layered superlattice approximation. Four fictitious hydrogen atoms with a charge of 0.5 electrons each are added for closing dangling Se bonds on the opposite side of the film. Ab initio calculations are performed using the QUANTUM ESPRESSO software based on the density functional theory. It is shown that relaxation results in splitting of atomic layers. We calculate and analyze the band structures and total and layer-wise densities of electron states for four variants of the surface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

A half century of density functional theory

Today’s most popular method for calculating the electronic structure of atoms, molecules, liquids, solids, and plasmas began as a bold hypothesis: The electron density distribution completely characterizes the ground state of a many-electron system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Syntheses, crystal structure, and electronic properties of the five ABaMQ{sub 4} compounds RbBaPS{sub 4}, CsBaPS{sub 4}, CsBaVS{sub 4}, RbBaVSe{sub 4}, and CsBaVSe{sub 4}

Five new compounds belonging to the ABaMQ{sub 4} family were synthesized by solid-state chemistry at 1123 K. The compounds RbBaPS{sub 4}, CsBaPS{sub 4}, CsBaVS{sub 4}, RbBaVSe{sub 4}, and CsBaVSe{sub 4} are isostructural and have the TlEuPS{sub 4} structure type. They crystallize in space group D{sup 16}{sub 2h} – Pnma of the orthorhombic system. Their structure consists isolated MQ{sub 4} tetrahedra separated by A and Ba atoms to form a salt-like structure. Density Functional Theory (DFT) calculations of the electronic structures with the use of the HSE functional suggest that the compounds are semiconductors with calculated band gaps of 3.3 eV (RbBaPS{sub 4}), 3.4 eV (CsBaPS{sub 4}), 2.3 eV (CsBaVS{sub 4}), and 1.6 eV (RbBaVSe{sub 4}). - Graphical abstract: General view of the ABaMQ{sub 4} structure down the a axis. - Highlights: • Five new ABaMQ{sub 4} compounds were synthesized by solid-state chemistry at 1123 K. • RbBaPS{sub 4}, CsBaPS{sub 4}, CsBaVS{sub 4}, RbBaVSe{sub 4}, and CsBaVSe{sub 4} have the TlEuPS{sub 4} structure type. • The compounds are semiconductors with calculated band gaps ranging from 1.6 to 3.4 eV.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Nb{sub 2}OsB{sub 2}, with a new twofold superstructure of the U{sub 3}Si{sub 2} type: Synthesis, crystal chemistry and chemical bonding

The new ternary metal-rich boride, Nb{sub 2}OsB{sub 2}, was synthesized by arc-melting the elements in a water-cooled copper crucible under an argon atmosphere. The compound was characterized from single-crystal X-ray data and EDX measurements. It crystallizes as a new superstructure (space group P4/mnc, no. 128) of the tetragonal U{sub 3}Si{sub 2}-structure type with lattice parameters a=5.922(1) Å and c=6.879(2) Å. All of the B atoms are involved in B{sub 2} dumbbells with B–B distances of 1.89(4) Å. Structure relaxation using VASP (Vienna ab intio Simulation Package) has confirmed the space group and the lattice parameters. According to electronic structure calculations (TB–LMTO–ASA), the homoatomic B–B interactions are optimized and very strong, but relatively strong heteroatomic Os–B, Nb–B and Nb–Os bonds are also found: These interactions, which together build a three-dimensional network, are mainly responsible for the structural stability of this new phase. The density of state at the Fermi level predicts metallic behavior, as expected, from this metal-rich boride. - Graphical abstract: Nb{sub 2}OsB{sub 2} is, to the best of our knowledge, the first fully characterized phase in the ternary Nb–Os–B system. It crystallizes (space group P4/mnc, 128) with a new twofold superstructure of the U{sub 3}Si{sub 2} structure type (space group P4/mbm, 127), and is therefore the first boride in this structure family crystallizing with a superstructure of the U{sub 3}Si{sub 2} structure type. We show that the distortions leading to this superstructure occurs mainly in the Nb-layer, which tries to accommodate the large osmium atoms. The consequence of this puckering is the building osmium dumbbells instead of chains along [001]. - Highlights: • First compound in the Nb–Os–B system. • New twofold superstructure of U{sub 3}Si{sub 2} structure type. • Puckering of Nb-layer responsible for superstructure occurrence. • Chemical bonding studied by density functional theory.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Featureless adaptive optimization accelerates functional electronic materials design

Electronic materials that exhibit phase transitions between metastable states (e.g., metal-insulator transition materials with abrupt electrical resistivity transformations) are challenging to decode. For these materials, conventional machine learning methods display limited predictive capability due to data scarcity and the absence of features that impede model training. In this article, we demonstrate a discovery strategy based on multi-objective Bayesian optimization to directly circumvent these bottlenecks by utilizing latent variable Gaussian processes combined with high-fidelity electronic structure calculations for validation in the chalcogenide lacunar spinel family. We directly and simultaneously learn phase stability and bandgap tunability from chemical composition alone to efficiently discover all superior compositions on the design Pareto front. Previously unidentified electronic transitions also emerge from our featureless adaptive optimization engine. Our methodology readily generalizes to optimization of multiple properties, enabling co-design of complex multifunctional materials, especially where prior data is sparse.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Aces4: A Platform for Computational Chemistry Calculations with Extremely Large Block-Sparse Arrays

Aces4 is a parallel programming platform comprising a DSL for Computational Chemistry and its runtime system. It offers a convenient way to express parallelism together with extensive support for extremely large, possibly sparse, distributed arrays. It aids scientists in the creation of performant, scalable, massively parallel programs that can effectively take advantage of leadership class computing systems to address important scientific questions. Aces4 has enabled the development and implementation of new methods in electronic structure theory which are breaking new ground in their ability to perform highly accurate calculations on ever larger molecular systems. In this paper the design of Aces4, which is based on the the Super Instruction Architecture approach, is described. Experimental scaling results for Molecular Cluster Perturbation Theory, a new method enabled by Aces4, and CCSD, a widely used computational chemistry method are given.

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

Pressure induced magnetic phase transition in RhFe{sub 3}N and IrFe{sub 3}N: An ab-initio study

The structural, electronic, elastic and magnetic properties of RhFe{sub 3}N and IrFe{sub 3}N are investigated using ab-initio calculations based on density functional theory as implemented in VASP code within the gradient generalized approximation. The non-spin polarized and spin polarized calculations are performed for these nitrides at normal and high pressures. It is found that these ternary nitrides are stable in ferromagnetic state at normal pressure. The lattice constant and bulk modulus values are calculated. The electronic structure reveals that these nitrides are metallic at normal pressure. The calculated elastic constants indicate that they are mechanically stable at ambient pressure. Ferromagnetic to nonmagnetic phase transition is observed in RhFe{sub 3}N and IrFe{sub 3}N at high pressure. Ferromagnetism is quenched in these nitrides at high pressure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Electronic structure and magnetic properties of zigzag blue phosphorene nanoribbons

We investigated the electronic structure and magnetism of zigzag blue phosphorene nanoribbons (ZBPNRs) using first principles density functional theory calculations by changing the widths of ZBPNRs from 1.5 to 5 nm. In addition, the effect of H and O passivation was explored as well. The ZBPNRs displayed intra-edge antiferromagnetic ground state with a semiconducting band gap of ∼0.35 eV; and this was insensitive to the edge structure relaxation effect. However, the edge magnetism of ZBPNRs disappeared with H-passivation. Moreover, the band gap of H-passivated ZBPNRs was greatly enhanced because the calculated band gap was ∼1.77 eV, and this was almost the same as that of two-dimensional blue phosphorene layer. For O-passivated ZBPNRs, we also found an intra-edge antiferromagnetic state. Besides, both unpassivated and O-passivated ZBPNRs preserved almost the same band gap. We predict that the electronic band structure and magnetic properties can be controlled by means of passivation. Moreover, the edge magnetism can be also modulated by the strain. Nonetheless, the intrinsic physical properties are size independent. This feature can be an advantage for device applications because it may not be necessary to precisely control the width of the nanoribbon.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

First-principles calculation on β-SiC(111)/α-WC(0001) interface

The α-WC(0001) surface and β-SiC(111)/α-WC(0001) interface were studied by first-principles calculation based on density functional theory. It is demonstrated that the α-WC(0001) surface models with more than nine atom-layers exhibit bulk-like interior, wherein the surface relaxations localized within the top three layers are well converged. Twenty-four specific geometry models of SiC/WC interface structures with different terminations and stacking sites were chosen. The calculated work of adhesion and interface energy suggest that the most stable interface structure has the C-C bonding across the interface, yielding the largest work of adhesion and the lowest interface energy. Moreover, the top-site stacking sequence is preferable for the C/C-terminated interface. The effects of the interface on the electronic structures of the C/C-terminated interfaces are mainly localized within the first and second layers of the interface. Calculations of the work of adhesion and interface energy provide theoretical evidence that the mechanical failure may initiate at the interface or in SiC but not in WC.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

First principles study of electronic structure for cubane-like and ring-shaped structures of M{sub 4}O{sub 4}, M{sub 4}S{sub 4} clusters (M = Mn, Fe, Co, Ni, Cu)

Spin-polarized DFT has been used to perform a comparative study of the geometric structures and electronic properties for isolated M{sub 4}X{sub 4} nano clusters between their two stable isomers - a planar rhombus-like 2D structure and a cubane-like 3D structure with M = Mn, Fe, Co, Ni, Cu ; X = O, S. These two structural patterns of the M{sub 4}X{sub 4} clusters are commonly found as building blocks in several poly-nuclear transition metal complexes in inorganic chemistry. The effects of the van der Waals corrections to the physical properties have been considered in the electronic structure calculations employing the empirical Grimme’s correction (DFT+D2). We report here an interesting trend in their relative structural stability - the isolated M{sub 4}O{sub 4} clusters prefer to stabilize more in the planar structure, while the cubane-like 3D structure is more favorable for most of the isolated M{sub 4}S{sub 4} clusters than their planar 2D counterparts. Our study reveals that this contrasting trend in the relative structural stability is expected to be driven by an interesting interplay between the s-d and p-d hybridization effects of the constituents’ valence electrons.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Band gap engineering of MoS{sub 2} upon compression

Molybdenum disulfide (MoS{sub 2}) is a promising candidate for 2D nanoelectronic devices, which shows a direct band-gap for monolayer structure. In this work we study the electronic structure of MoS{sub 2} upon both compressive and tensile strains with first-principles density-functional calculations for different number of layers. The results show that the band-gap can be engineered for experimentally attainable strains (i.e., ±0.15). However, compressive strain can result in bucking that can prevent the use of large compressive strain. We then studied the stability of the compression, calculating the critical strain that results in the on-set of buckling for free-standing nanoribbons of different lengths. The results demonstrate that short structures, or few-layer MoS{sub 2}, show semi-conductor to metal transition upon compressive strain without bucking.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Electronic structure of ferromagnetic semiconductor material on the monoclinic and rhombohedral ordered double perovskites La{sub 2}FeCoO{sub 6}

Double perovskite La{sub 2}FeCoO{sub 6} with monoclinic structure and rhombohedra structure show as ferromagnetic semiconductor based on density functional theory calculation. The ferromagnetic semiconductor state can be well explained by the superexchange interaction. Moreover, the ferromagnetic semiconductor state remains under the generalized gradient approximation (GGA) and GGA plus onsite Coulomb interaction calculation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

A two-directional vibrational probe reveals different electric field orientations in solution and an enzyme active site

We report the catalytic power of an electric field depends on its magnitude and orientation with respect to the reactive chemical species. Understanding and designing new catalysts for electrostatic catalysis thus requires methods to measure the electric field orientation and magnitude at the molecular scale. We demonstrate that electric field orientations can be extracted using a two-directional vibrational probe by exploiting the vibrational Stark effect of both the C=O and C–D stretches of a deuterated aldehyde. Combining spectroscopy with molecular dynamics and electronic structure partitioning methods, we demonstrate that, despite distinct polarities, solvents act similarly in their preference for electrostatically stabilizing large bond dipoles at the expense of destabilizing small ones. In contrast, we find that for an active-site aldehyde inhibitor of liver alcohol dehydrogenase, the electric field orientation deviates markedly from that found in solvents, which provides direct evidence for the fundamental difference between the electrostatic environment of solvents and that of a preorganized enzyme active site.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Exchange interaction in hexagonal MnRhP from first-principles studies

Electronic structure and magnetic properties for MnRhP have been studied from a first-principles density functional calculation. The calculated lattice constants, a = 6.228 Å and c = 3.571 Å, are in good agreement with the experimental values of a = 6.223 Å and c = 3.585 Å. The calculated moment of Mn is 3.1 μ{sub B}/atom, resulting in a total moment of 3.0 μ{sub B}/atom due to small moments induced at Rh and P sites. The magnetic moment of Mn decreases with unit cell size. The exchange interactions are dominated by positive Mn-Mn exchange coupling (J{sub Mn−Mn}), implying a stable ferromagnetic ordering in Mn sublattice. In particular, J{sub Mn−Mn} shows a maximum value (1.5 mRy) at the the optimized unit cell size. The structural distortion or unit cell size change will affect J{sub Mn−Mn}, which is intimately related to the magneto-elastic and magneto-caloric effect.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

A first-principles study on new high-pressure metastable polymorphs of MoO{sub 2}

The pressure-dependence of the stabilities of several MoO{sub 2} phases has been investigated by density-functional theory (GGA/PBE/PAW). Out of a set of 15 MX{sub 2} structures, the [SnO{sub 2}(II)], [α-PbO{sub 2}], and a modified rutile structure type were identified as possible metastable MoO{sub 2} polymorphs based on the analysis of thermodynamic properties and dynamic stability. High-pressure calculations suggest an orthorhombic TiO{sub 2} structure, dubbed [ortho-TiO{sub 2}], as a high-pressure polymorph at around 25 GPa. Furthermore, we find that the previously reported rutile-type MoO{sub 2} may be understood as a modified rutile type similar to the [VO{sub 2}] structure. - Graphical abstract: First-principles electronic structure and thermochemical calculations reveal four structure candidates as possible metastable polymorphs of MoO{sub 2}. Most promising is a distorted rutile-type similar to the known [VO{sub 2}] structure. An orthorhombic polymorph is proposed as a high-pressure polymorph. Display Omitted - Highlights: • Three possible metastable structure candidates for MoO{sub 2}. • Undistorted rutile type is improbable, a new distorted rutile-type MoO{sub 2} was suggested. • Orthorhombic phase of MoO{sub 2} (ortho-TiO{sub 2} type) should form at 25 GPa. • ab initio thermochemical data provided for MoO{sub 2}.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2011

Imaging Local Electronic Corrugations and Doped Regions in Graphene

Electronic structure heterogeneities are ubiquitous in two-dimensional graphene and profoundly impact the transport properties of this material. Here we show the mapping of discrete electronic domains within a single graphene sheet using scanning transmission X-ray microscopy in conjunction with ab initio density functional theory calculations. Scanning transmission X-ray microscopy imaging provides a wealth of detail regarding the extent to which the unoccupied levels of graphene are modified by corrugation, doping and adventitious impurities, as a result of synthesis and processing. Local electronic corrugations, visualized as distortions of the {pi}*cloud, have been imaged alongside inhomogeneously doped regions characterized by distinctive spectral signatures of altered unoccupied density of states. The combination of density functional theory calculations, scanning transmission X-ray microscopy imaging, and in situ near-edge X-ray absorption fine structure spectroscopy experiments also provide resolution of a longstanding debate in the literature regarding the spectral assignments of pre-edge and interlayer states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗