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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 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

First-principles binary diffusion coefficients for H, H 2 and four normal alkanes + N 2

Collision integrals related to binary (dilute gas) diffusion are calculated classically for six species colliding with N 2 . The most detailed calculations make no assumptions regarding the complexity of the potential energy surface, and the resulting classical collision integrals are in excellent agreement with previous semiclassical results for H + N 2 and H 2 + N 2 and with recent experimental results for C n H 2n+2 + N 2 , n = 2–4. The detailed classical results are used to test the accuracy of three simplifying assumptions typically made when calculating collision integrals: (1) approximating the intermolecular potential as isotropic, (2) neglecting the internal structure of the colliders (i.e., neglecting inelasticity), and (3) employing unphysical R –12 repulsive interactions. The effect of anisotropy is found to be negligible for H + N 2 and H 2 + N 2 (in agreement with previous quantum mechanical and semiclassical results for systems involving atomic and diatomic species) but is more significant for larger species at low temperatures. For example, the neglect of anisotropy decreases the diffusion coefficient for butane + N 2 by 15% at 300 K. The neglect of inelasticity, in contrast, introduces only very small errors. Approximating the repulsive wall as an unphysical R –12 interaction is a significant source of error at all temperatures for the weakly interacting systems H + N 2 and H 2 + N 2 , with errors as large as 40%. For the normal alkanes in N 2 , which feature stronger interactions, the 12/6 Lennard–Jones approximation is found to be accurate, particularly at temperatures above –700 K where it predicts the full-dimensional result to within 5% (although with somewhat different temperature dependence). Overall, the typical practical approach of assuming isotropic 12/6 Lennard–Jones interactions is confirmed to be suitable for combustion applications except for weakly interacting systems, such as H + N 2 . For these systems, anisotropy and inelasticity can safely be neglected but a more detailed description of the repulsive wall is required for quantitative predictions. Moreover, a straightforward approach for calculating effective isotropic potentials with realistic repulsive walls is described. An analytic expression for the calculated diffusion coefficient for H + N 2 is presented and is estimated to have a 2-sigma error bar of only 0.7%.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

First principles assessment of helium trapping in Y{sub 2}TiO{sub 5} in nano-featured ferritic alloys

Nano-scale Y{sub 2}Ti{sub 2}O{sub 7} and Y{sub 2}TiO{sub 5} oxides are the major features that provide high strength and irradiation tolerance in nano-structured ferritic alloys. Here, we employ density functional theory to study helium trapping in Y{sub 2}TiO{sub 5}. The results suggest that helium is more deeply trapped in Y{sub 2}TiO{sub 5} compared to Y{sub 2}Ti{sub 2}O{sub 7}. Helium occupies open channels in Y{sub 2}TiO{sub 5}, where it weakly chemically interacts with neighboring oxygen anions, and results in less volume expansion compared to Y{sub 2}Ti{sub 2}O{sub 7}, reducing strains in the iron matrix. The corresponding helium mobility in these channels is very high. While its ultimate fate is to form oxide/matrix interface bubbles, transient deep trapping of helium in oxides plays a major role in the ability of NFA to manage helium distribution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Semiclassical Monte Carlo: A first principles approach to non-adiabatic molecular dynamics

Modeling the dynamics of photophysical and (photo)chemical reactions in extended molecular systems is a new frontier for quantum chemistry. Many dynamical phenomena, such as intersystem crossing, non-radiative relaxation, and charge and energy transfer, require a non-adiabatic description which incorporate transitions between electronic states. Additionally, these dynamics are often highly sensitive to quantum coherences and interference effects. Several methods exist to simulate non-adiabatic dynamics; however, they are typically either too expensive to be applied to large molecular systems (10's-100's of atoms), or they are based on ad hoc schemes which may include severe approximations due to inconsistencies in classical and quantum mechanics. We present, in detail, an algorithm based on Monte Carlo sampling of the semiclassical time-dependent wavefunction that involves running simple surface hopping dynamics, followed by a post-processing step which adds little cost. The method requires only a few quantities from quantum chemistry calculations, can systematically be improved, and provides excellent agreement with exact quantum mechanical results. Here we show excellent agreement with exact solutions for scattering results of standard test problems. Additionally, we find that convergence of the wavefunction is controlled by complex valued phase factors, the size of the non-adiabatic coupling region, and the choice of sampling function. These results help in determining the range of applicability of the method, and provide a starting point for further improvement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

First-order derivative couplings between excited states from adiabatic TDDFT response theory

We present a complete derivation of derivative couplings between excited states in the framework of adiabatic time-dependent density functional response theory. Explicit working equations are given and the resulting derivative couplings are compared with derivative couplings from a pseudo-wavefunction ansatz. For degenerate excited states, i.e., close to a conical intersection (CI), the two approaches are identical apart from an antisymmetric overlap term. However, if the difference between two excitation energies equals another excitation energy, the couplings from response theory exhibit an unphysical divergence. This spurious behavior is a result of the adiabatic or static kernel approximation of time-dependent density functional theory leading to an incorrect analytical structure of the quadratic response function. Numerical examples for couplings close to a CI and for well-separated electronic states are given.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

First experiments probing the collision of parallel magnetic fields using laser-produced plasmas

Novel experiments to study the strongly-driven collision of parallel magnetic fields in β ∼ 10, laser-produced plasmas have been conducted using monoenergetic proton radiography. These experiments were designed to probe the process of magnetic flux pileup, which has been identified in prior laser-plasma experiments as a key physical mechanism in the reconnection of anti-parallel magnetic fields when the reconnection inflow is dominated by strong plasma flows. In the present experiments using colliding plasmas carrying parallel magnetic fields, the magnetic flux is found to be conserved and slightly compressed in the collision region. Two-dimensional (2D) particle-in-cell simulations predict a stronger flux compression and amplification of the magnetic field strength, and this discrepancy is attributed to the three-dimensional (3D) collision geometry. Future experiments may drive a stronger collision and further explore flux pileup in the context of the strongly-driven interaction of magnetic fields.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

First principles-based multiparadigm, multiscale strategy for simulating complex materials processes with applications to amorphous SiC films

Progress has recently been made in developing reactive force fields to describe chemical reactions in systems too large for quantum mechanical (QM) methods. In particular, ReaxFF, a force field with parameters that are obtained solely from fitting QM reaction data, has been used to predict structures and properties of many materials. Important applications require, however, determination of the final structures produced by such complex processes as chemical vapor deposition, atomic layer deposition, and formation of ceramic films by pyrolysis of polymers. This requires the force field to properly describe the formation of other products of the process, in addition to yielding the final structure of the material. We describe a strategy for accomplishing this and present an example of its use for forming amorphous SiC films that have a wide variety of applications. Extensive reactive molecular dynamics (MD) simulations have been carried out to simulate the pyrolysis of hydridopolycarbosilane. The reaction products all agree with the experimental data. After removing the reaction products, the system is cooled down to room temperature at which it produces amorphous SiC film, for which the computed radial distribution function, x-ray diffraction pattern, and the equation of state describing the three main SiC polytypes agree with the data and with the QM calculations. Extensive MD simulations have also been carried out to compute other structural properties, as well the effective diffusivities of light gases in the amorphous SiC film.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Ba{sub 2}TeO as an optoelectronic material: First-principles study

The band structure, optical, and defects properties of Ba{sub 2}TeO are systematically investigated using density functional theory with a view to understanding its potential as an optoelectronic or transparent conducting material. Ba{sub 2}TeO crystallizes with tetragonal structure (space group P4/nmm) and with a 2.93 eV optical bandgap [Besara et al., J. Solid State Chem. 222, 60 (2015)]. We find relatively modest band masses for both electrons and holes suggesting applications. Optical properties show infrared-red absorption when doped. This could potentially be useful for combining wavelength filtering and transparent conducting functions. Furthermore, our defect calculations show that Ba{sub 2}TeO is intrinsically p-type conducting under Ba-poor condition. However, the spontaneous formation of the donor defects may constrain the p-type transport properties and would need to be addressed to enable applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

A first-principles study of cementite (Fe{sub 3}C) and its alloyed counterparts: Elastic constants, elastic anisotropies, and isotropic elastic moduli

A comprehensive computational study of elastic properties of cementite (Fe{sub 3}C) and its alloyed counterparts (M{sub 3}C (M = Al, Co, Cr, Cu, Fe, Hf, Mn, Mo, Nb, Ni, Si, Ta, Ti, V, W, Zr, Cr{sub 2}FeC and CrFe{sub 2}C) having the crystal structure of Fe{sub 3}C is carried out employing electronic density-functional theory (DFT), all-electron PAW pseudopotentials and the generalized gradient approximation for the exchange-correlation energy (GGA). Specifically, as a part of our systematic study of cohesive properties of solids and in the spirit of materials genome, following properties are calculated: (i) single-crystal elastic constants, C{sub ij}, of above M{sub 3}Cs; (ii) anisotropies of bulk, Young’s and shear moduli, and Poisson’s ratio based on calculated C{sub ij}s, demonstrating their extreme anisotropies; (iii) isotropic (polycrystalline) elastic moduli (bulk, shear, Young’s moduli and Poisson’s ratio) of M{sub 3}Cs by homogenization of calculated C{sub ij}s; and (iv) acoustic Debye temperature, θ{sub D}, of M{sub 3}Cs based on calculated C{sub ij}s. We provide a critical appraisal of available data of polycrystalline elastic properties of alloyed cementite. Calculated single crystal properties may be incorporated in anisotropic constitutive models to develop and test microstructure-processing-property-performance links in multi-phase materials where cementite is a constituent phase.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Quantitative first-principles theory of interface absorption in multilayer heterostructures

The unique chemical bonds and electronic states of interfaces result in optical properties that are different from those of the constituting bulk materials. In the nanoscale regime, the interface effects can be dominant and impact the optical response of devices. Using density functional theory (DFT), the interface effects can be calculated, but DFT is computationally limited to small systems. In this paper, we describe a method to combine DFT with macroscopic methodologies to extract the interface effect on absorption in a consistent and quantifiable manner. The extracted interface effects are an independent parameter and can be applied to more complicated systems. Finally, we demonstrate, using NiSi 2 /Si heterostructures, that by varying the relative volume fractions of interface and bulk, we can tune the spectral range of the heterostructure absorption.

36 MATERIALS SCIENCE↗
DOE OSTI2015

The high pressure structure and equation of state of 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) up to 20 GPa: X-ray diffraction measurements and first principles molecular dynamics simulations

Recent theoretical studies of 2,6-diamino-3,5-dinitropyrazine-1-oxide (C{sub 4}H{sub 4}N{sub 6}O{sub 5} Lawrence Livermore Molecule No. 105, LLM-105) report unreacted high pressure equations of state that include several structural phase transitions, between 8 and 50 GPa, while one published experimental study reports equation of state (EOS) data up to a pressure of 6 GPa with no observed transition. Here we report the results of a synchrotron-based X-ray diffraction study and also ambient temperature isobaric-isothermal atomistic molecular dynamics simulations of LLM-105 up to 20 GPa. We find that the ambient pressure phase remains stable up to 20 GPa; there is no indication of a pressure induced phase transition. We do find a prominent decrease in b-axis compressibility starting at approximately 13 GPa and attribute the stiffening to a critical length where inter-sheet distance becomes similar to the intermolecular distance within individual sheets. The ambient temperature isothermal equation of state was determined through refinements of measured X-ray diffraction patterns. The pressure-volume data were fit using various EOS models to yield bulk moduli with corresponding pressure derivatives. We find very good agreement between the experimental and theoretically derived EOS.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Structure sensitivity in oxide catalysis: First-principles kinetic Monte Carlo simulations for CO oxidation at RuO{sub 2}(111)

We present a density-functional theory based kinetic Monte Carlo study of CO oxidation at the (111) facet of RuO{sub 2}. We compare the detailed insight into elementary processes, steady-state surface coverages, and catalytic activity to equivalent published simulation data for the frequently studied RuO{sub 2}(110) facet. Qualitative differences are identified in virtually every aspect ranging from binding energetics over lateral interactions to the interplay of elementary processes at the different active sites. Nevertheless, particularly at technologically relevant elevated temperatures, near-ambient pressures and near-stoichiometric feeds both facets exhibit almost identical catalytic activity. These findings challenge the traditional definition of structure sensitivity based on macroscopically observable turnover frequencies and prompt scrutiny of the applicability of structure sensitivity classifications developed for metals to oxide catalysis.

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

First principles calculations of point defect diffusion in CdS buffer layers: Implications for Cu(In,Ga)(Se,S){sub 2} and Cu{sub 2}ZnSn(Se,S){sub 4}-based thin-film photovoltaics

We investigate point defects in CdS buffer layers that may arise from intermixing with Cu(In,Ga)Se{sub 2} (CIGSe) or Cu{sub 2}ZnSn(S,Se){sub 4} (CZTSSe) absorber layers in thin-film photovoltaics (PV). Using hybrid functional calculations, we characterize the migration barriers of Cu, In, Ga, Se, Sn, Zn, Na, and K impurities and assess the activation energies necessary for their diffusion into the bulk of the buffer. We find that Cu, In, and Ga are the most mobile defects in CIGS-derived impurities, with diffusion expected to proceed into the buffer via interstitial-hopping and cadmium vacancy-assisted mechanisms at temperatures ∼400 °C. Cu is predicted to strongly favor migration paths within the basal plane of the wurtzite CdS lattice, which may facilitate defect clustering and ultimately the formation of Cu-rich interfacial phases as observed by energy dispersive x-ray spectroscopic elemental maps in real PV devices. Se, Zn, and Sn defects are found to exhibit much larger activation energies and are not expected to diffuse within the CdS bulk at temperatures compatible with typical PV processing temperatures. Lastly, we find that Na interstitials are expected to exhibit slightly lower activation energies than K interstitials despite having a larger migration barrier. Still, we find both alkali species are expected to diffuse via an interstitially mediated mechanism at slightly higher temperatures than enable In, Ga, and Cu diffusion in the bulk. Our results indicate that processing temperatures in excess of ∼400 °C will lead to more interfacial intermixing with CdS buffer layers in CIGSe devices, and less so for CZTSSe absorbers where only Cu is expected to significantly diffuse into the buffer.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Experimental evidence for pressure-induced first order transition in cerium nitride from B1 to B10 structure type

Here, the crystal structure of CeN was investigated up to pressures of 82 GPa, using diamond anvil cell powder X-ray diffraction in two experiments with He and Si-oil as the pressure transmitting media. In contrast to previous reports, we do not observe the B2 (CsCl type) structure at high pressure. Instead, the structural phase transition, starting at 65 GPa, from the ambient rock salt B1 structure results in a distorted CsCl-like B10 structure, irrespective of the pressure medium. Our result unambiguously confirms two recent density functional theory (DFT) studies predicting the B10 phase to be stable at these pressures, rather than the B2 (CsCl type) phase previously reported. The B10 structure appears to approach the B2 structure as pressure is increased further, but DFT calculations indicate that an L1 0 structure (AuCu type) is energetically favored

36 MATERIALS SCIENCE↗
DOE OSTI2018

Motional Stark effect imaging first results on the DIII-D tokamak

A motional Stark effect (MSE) imaging diagnostic was benchmarked against existing conventional MSE polarimeters on the DIII-D tokamak and delivered new capabilities for measuring the magnetic pitch angle from 2 neutral beams and on the high field side of DIII-D. Line integration across flux surfaces was considerable for the radial view utilised; yet, the imaging MSE measurements from both beams were self-consistent and in close agreement with conventional MSE measurements. The ferroelectric liquid crystal waveplate used in the imaging polarimeter was discovered to have spatially non-uniform retardance; thus, it is required for the calibration source to replicate the ray paths of the neutral beam emission through the optical system.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2013

EXTRAGALACTIC BACKGROUND LIGHT FROM HIERARCHICAL GALAXY FORMATION: GAMMA-RAY ATTENUATION UP TO THE EPOCH OF COSMIC REIONIZATION AND THE FIRST STARS

We present a new model of the extragalactic background light (EBL) and corresponding {gamma}{gamma} opacity for intergalactic gamma-ray absorption from z = 0 up to z = 10, based on a semi-analytical model of hierarchical galaxy formation that reproduces key observed properties of galaxies at various redshifts. Including the potential contribution from Population III stars and following the cosmic reionization history in a simplified way, the model is also broadly consistent with available data concerning reionization, particularly the Thomson scattering optical depth constraints from Wilkinson Microwave Anisotropy Probe (WMAP). In comparison with previous EBL studies up to z {approx} 3-5, our predicted {gamma}{gamma} opacity is in general agreement for observed gamma-ray energy below 400/(1 + z) GeV, whereas it is a factor of {approx}2 lower above this energy because of a correspondingly lower cosmic star formation rate, even though the observed ultraviolet (UV) luminosity is well reproduced by virtue of our improved treatment of dust obscuration and direct estimation of star formation rate. The horizon energy at which the gamma-ray opacity is unity does not evolve strongly beyond z {approx} 4 and approaches {approx}20 GeV. The contribution of Population III stars is a minor fraction of the EBL at z = 0, and is also difficult to distinguish through gamma-ray absorption in high-z objects, even at the highest levels allowed by the WMAP constraints. Nevertheless, the attenuation due to Population II stars should be observable in high-z gamma-ray sources by telescopes such as Fermi or the Cherenkov Telescope Array and provide a valuable probe of the evolving EBL in the rest-frame UV. The detailed results of our model are publicly available in numerical form at http://www.slac.stanford.edu/{approx}yinoue/Download.html.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

First frontier field constraints on the cosmic star formation rate density AT z ~ 10—the impact of lensing shear on completeness of high-redshift galaxy samples

In this work, we search the complete Hubble Frontier Field data set of Abell 2744 and its parallel field for $z\sim 10$ sources to further refine the evolution of the cosmic star formation rate density (SFRD) between $z\sim 8$ and $z\sim 10$. We independently confirm two images of the recently discovered triply imaged $z\sim 9.8$ source by Zitrin et al. and set an upper limit for similar $z\sim 10$ galaxies with red colors of ${J}_{125}-{H}_{160}\gt 1.2$ in the parallel field of Abell 2744. We utilize extensive simulations to derive the effective selection volume of Lyman-break galaxies at $z\sim 10$, both in the lensed cluster field and in the adjacent parallel field. Particular care is taken to include position-dependent lensing shear to accurately account for the expected sizes and morphologies of highly magnified sources. We show that both source blending and shear reduce the completeness at a given observed magnitude in the cluster, particularly near the critical curves. These effects have a significant, but largely overlooked, impact on the detectability of high-redshift sources behind clusters, and substantially reduce the expected number of highly magnified sources. The detections and limits from both pointings result in an SFRD which is consistent within the uncertainties with previous estimates at $z\sim 10$ from blank fields. The combination of these new results with all other estimates is also consistent with a rapidly declining SFRD in the 170 Myr from $z\sim 8$ to $z\sim 10$ as predicted by cosmological simulations and dark-matter halo evolution in ΛCDM. Once biases introduced by magnification-dependent completeness are accounted for, the full six cluster and parallel Frontier Field program will be an extremely powerful new data set to probe the evolution of the galaxy population at $z\gt 8$ before the advent of the James Webb Space Telescope.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

The interaction of the ITER first wall with magnetic perturbations

Mitigation of the multiple risks associated with disruptions and runaway electrons in tokamaks involves competing demands. Success requires that each risk be understood sufficiently that appropriate compromises can be made. Here the focus is on the interaction of short timescale magnetic-perturbations with the structure in ITER that is closest to the plasma, blanket modules covered by separated beryllium tiles. The effect of this tiled surface on the perturbations and on the forces on structures is subtle. Indeterminacy can be introduced by tile-to-tile shorting. A determinate subtlety is introduced because electrically separated tiles can act as a conducting surface for magnetic perturbations that have a normal component to the surface. A practical method for including this determinate subtlety into plasma simulations is developed. The shorter the timescales and the greater the localization, particularly in the toroidal direction, the more important the magnetic effects of the tiles become.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗