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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
NASA NTRS1985

Size and DNA distributions of electrophoretically separated cultured human kidney cells

Electrophoretic purification of purifying cultured cells according to function presumes that the size of cycle phase of a cell is not an overriding determinant of its electrophoretic velocity in an electrophoretic separator. The size distributions and DNA distributions of fractions of cells purified by density gradient electrophoresis were determined. No systematic dependence of electrophoretic migration upward in a density gradient column upon either size or DNA content were found. It was found that human leukemia cell populations, which are more uniform function and found in all phases of the cell cycle during exponential growth, separated on a vertical sensity gradient electrophoresis column according to their size, which is shown to be strictly cell cycle dependent.

Kunze, M. E.↗
DOE OSTI2025

Free-energy orbital-free density functional theory: recent developments, perspective, and outlook

By summarizing the constraint-based development of orbital-free free-energy density functional approximations, we provide a perspective on progress over the last 15 years, the limitations of existing functionals, and the challenges awaiting resolution. We outline the chronology of the development of noninteracting and exchange-correlation free-energy orbital-free functionals and summarize the theoretical basis of existing local density approximation, second-order approximation, generalized gradient approximation (GGA), and meta-GGAs. We discuss limitations and challenges such as problems with thermodynamic derivatives, free-energy nonadditivity and the closely related issue of all-electron versus valence-only local pseudo-potential performance.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS2019

Effects of Topography on Tropical Forest Structure Depend on Climate Context

Topography affects abiotic conditions which can influence the structure, function, and dynamics of ecological communities. An increasing number of studies have demonstrated biological consequences of fine-scale topographic heterogeneity but we have a limited understanding of how We merged high-resolution (1 sq. meter) data on topography and canopy height derived from airborne lidar with ground-based data from 15 forest plots in Puerto Rico distributed along a precipitation gradient spanning ca. 800 to 3,500 mm yr(exp -1). Ground-based data included species composition, estimated above-ground biomass (AGB), and two key functional traits (wood density and leaf mass per area, LMA) that reflect resource-use strategies and a trade-off between hydraulic safety and hydraulic efficiency. We used hierarchical Bayesian models to evaluate how the interaction between topography climate is related to metrics of forest structure (i.e., canopy height and AGB), as well as taxonomic and functional alpha- and beta-diversity. Fine-scale topography (characterized with the topographic wetness index, TWI) significantly affected forest structure and the strength (and in some cases direction) of these effects varied across the precipitation gradient. In all plots, canopy height increased with topographic wetness but the effect was much stronger in dry compared to wet forest plots. In dry forest plots, topographically wetter microsites also had higher levels of AGB but in wet forest plots, topographically drier microsites had higher AGB. Fine-scale topography influenced functional composition but had only weak or non-significant effects on taxonomic and functional alpha- and beta-diversity. For instance, community-weighted wood density followed a similar pattern to AGB across plots. We also found a marginally significant association between variation of wood density and topographic heterogeneity that depended on climate context. Synthesis: The effects of fine-scale topographic heterogeneity on tropical forest structure and composition depend on the climate context. Our study demonstrates how a stronger integration of topographic heterogeneity across precipitation gradients could improve estimates of forest structure and biomass, and may provide insight to the ways that topography might mediate species responses to drought and climate change.

Tropical dry forest↗
DOE OSTI2021

Examination of How Well Long-Range-Corrected Density Functionals Satisfy the Ionization Energy Theorem

For this work, we calculated the vertical ionization energies (VIE) of 99 species in two ways to examine the accuracy of several long-range-corrected (LC) hybrid meta functionals in comparison with a gradient approximation (GA), global hybrids, and doubly hybrids. In the category of LC functionals, we examined both those with meta ingredients (i.e., that depend on the kinetic energy density) and those without them. The LC-hybrid meta functionals examined are M11, revM11, M11plus, and ωB97M-V. The reference data used to assess accuracy consist of 95 molecules and 4 atoms in the GW100 set. The two methods studied are the ΔSCF method (involving the difference of neutral and cation self-consistent field (SCF) energies) and the ionization energy theorem (involving the orbital energy of the highest occupied molecular orbital, HOMO). We calculated linear correlation coefficients (r 2 ) and mean absolute deviations (MADs) between each approach and the reference VIE value from the CCSD(T)/def2-TZVPP level of theory. We compared the new LC-hybrid meta calculations to calculations with the 10 functionals in a previous VIE study by Brémond et al. and to the calculations with LC-BLYP (LC-Becke, Lee–Yang–Parr), CAM-B3LYP (Coulomb-attenuating-method Becke-3-parameter Lee–Yang–Parr), LC-ωHPBE, and ωB97X-D. The results show that Minnesota LC-hybrid meta functionals have the smallest mean absolute deviation of ionization energy theorem VIEs with the reference data; the LC-ωHPBE functional also does quite well in this test. This is very encouraging and indicates that LC-hybrid meta functionals would be the best starting points for the tuning strategy that has been shown to be a very good procedure for improving time-dependent density functional calculations, and it also helps explain the good success of LC-hybrid meta functionals for molecular excitation energies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Carbon nanotube thermoelectric devices by direct printing: Toward wearable energy converters

Thermoelectric devices convert thermal energy to electrical energy and are particularly well-suited for energy harvesting from waste heat. Even as the number of electronic devices used in daily life proliferates, technical advances diminish the average power such devices require to perform a given function. Here, localized thermal gradients that abound in our living environments, despite having modest energy densities, are therefore becoming increasingly viable and attractive to power such devices. With this motivation, we report the design, fabrication, and characterization of single-wall carbon nanotube thermoelectric devices (CNT-TDs) on flexible polyimide substrates as a basis for wearable energy converters. Our aqueous-solution-based film fabrication process could enable readily scalable, low-cost TDs; here, we demonstrate CNT-hydroxypropyl cellulose (HPC) composite thermoelectric films by aerosol jet printing. The electrical conductivity of the composite films is controlled through the number of CNT/HPC layers printed in combination with control of the annealing conditions.

30 DIRECT ENERGY CONVERSION↗
NASA NTRS2000

Influence of Mean-Density Gradient on Small-Scale Turbulence Noise

A physics-based methodology is described to predict jet-mixing noise due to small-scale turbulence. Both self- and shear-noise source teens of Lilley's equation are modeled and the far-field aerodynamic noise is expressed as an integral over the jet volume of the source multiplied by an appropriate Green's function which accounts for source convection and mean-flow refraction. Our primary interest here is to include transverse gradients of the mean density in the source modeling. It is shown that, in addition to the usual quadrupole type sources which scale to the fourth-power of the acoustic wave number, additional dipole and monopole sources are present that scale to lower powers of wave number. Various two-point correlations are modeled and an approximate solution to noise spectra due to multipole sources of various orders is developed. Mean flow and turbulence information is provided through RANS-k(epsilon) solution. Numerical results are presented for a subsonic jet at a range of temperatures and Mach numbers. Predictions indicated a decrease in high frequency noise with added heat, while changes in the low frequency noise depend on jet velocity and observer angle.

Khavaran, Abbas↗
DOE OSTI2023

Self-consistent implementation of locally scaled self-interaction-correction method

Recently proposed local self-interaction correction (LSIC) method is a one-electron self-interaction-correction (SIC) method that uses an iso-orbital indicator to apply the SIC at each point in space by scaling the exchange–correlation and Coulomb energy densities. The LSIC method is exact for the one-electron densities, also recovers the uniform electron gas limit of the uncorrected density functional approximation, and reduces to the well-known Perdew–Zunger SIC (PZSIC) method as a special case. This article presents the self-consistent implementation of the LSIC method using the ratio of Weizsäcker and Kohn–Sham kinetic energy densities as an iso-orbital indicator. The atomic forces as well as the forces on the Fermi-Löwdin orbitals are also implemented for the LSIC energy functional. Results show that LSIC with the simplest local spin density functional predicts atomization energies of the AE6 dataset better than some of the most widely used generalized-gradient-approximation (GGA) functional and barrier heights of the BH6 database better than some of the most widely used hybrid functionals. The LSIC method [a mean absolute error (MAE) of 0.008 Å] predicts bond lengths of a small set of molecules better than the PZSIC-LSDA (MAE 0.042 Å) and LSDA (0.011 Å). Furthermore, this work shows that accurate results can be obtained from the simplest density functional by removing the self-interaction-errors using an appropriately designed SIC method.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1999

Global Core Plasma Model

Abstract. The Global Core Plasma Model (GCPM) provides, empirically derived, core plasma density as a function of geomagnetic and solar conditions throughout the inner magnetosphere. It is continuous in value and gradient and is composed of separate models for the ionosphere, the plasmasphere, the plasmapause, the trough, and the polar cap. The relative composition of plasmaspheric H+, He+, and O+ is included in the GCPM. A blunt plasmaspheric bulge and rotation of the bulge with changing geomagnetic conditions is included. The GCPM is an amalgam of density models, intended to serve as a framework for continued improvement as new measurements become available and are used to characterize core plasma density, composition, and temperature.

Gallagher, Dennis L.↗
DOE OSTI2022

Laplacian-level meta-generalized gradient approximation for solid and liquid metals

In this work, we derive and motivate a Laplacian-level, orbital-free meta-generalized-gradient approximation (LL-MGGA) for the exchange-correlation energy, targeting accurate ground-state properties of sp and sd metallic condensed matter, in which the density functional for the exchange-correlation energy is only weakly nonlocal due to perfect long-range screening. Our model for the orbital-free kinetic energy density restores the fourth-order gradient expansion for exchange to the r 2 SCAN meta-GGA [Furness et al., J. Phys. Chem. Lett. 11, 8208 (2020)], yielding a LL-MGGA we call OFR2. OFR2 matches the accuracy of SCAN for prediction of common lattice constants and improves the equilibrium properties of alkali metals, transition metals, and intermetallics that were degraded relative to the PBE GGA values by both SCAN and r 2 SCAN. We compare OFR2 to the r 2 SCAN -L LL-MGGA [Mejia-Rodriguez and Trickey, Phys. Rev. B 102, 121109(R) (2020)] and show that OFR2 tends to outperform r 2 SCAN -L for the equilibrium properties of solids, but r 2 SCAN -L much better describes the atomization energies of molecules than OFR2 does. For best accuracy in molecules and nonmetallic condensed matter, we continue to recommend SCAN and r 2 SCAN. Numerical performance is discussed in detail, and our paper provides an outlook to machine learning.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Lattice Structure and Dynamics of Sparse Molecular Crystals: OsO 4 and RuO 4

OsO 4 and RuO 4 are molecular oxides with unique tetrameric structures and rare +8 oxidation states. Accurately modeling their properties remains challenging for density functional theory (DFT) due to weak intertetramer interactions, which standard functionals fail to capture. Here, in this work, we show that the van der Waals (vdW)-corrected density functional (vdW-DF-optB86b) provides structural parameters that are much closer to experimental values than the standard generalized gradient approximation, with volume predictions that fall within the experimentally observed range. Phonon band structure analysis shows that the inclusion of vdW interactions stabilizes soft phonon modes, highlighting the importance of dispersion corrections for accurate predictions of lattice dynamics. Experimental measurements of the phonon density of states for OsO 4 , obtained via inelastic neutron scattering, demonstrate good agreement with our vdW-DF-optB86b calculations. These results validate OsO 4 and RuO 4 as valuable benchmarks for structural and vibrational calculations via vdW-corrected DFT methods and offer insights for studying the broader class of sparse molecular materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Comparative Density Functional Theory Study of Magnetic Exchange Couplings in Dinuclear Transition-Metal Complexes

Multicenter transition-metal complexes (MCTMs) with magnetically interacting ions have been proposed as components for information-processing devices and storage units. For any practical application of MCTMs as magnetic units, it is crucial to characterize their magnetic behavior, and in particular, the isotropic magnetic exchange coupling, J, between its magnetic centers. Due to the large size of typical MCTMs, density functional theory is the only practical electronic structure method for evaluating the J coupling. Here, we assess the accuracy of different density functional approximations for predicting the magnetic couplings of eight dinuclear transition-metal complexes, including five dimanganese, two dicopper, and one divanadium with known reliable experimental J couplings spanning from ferromagnetic to strong antiferromagnetic. The density functionals considered include global hybrid functionals which mix semilocal density functional approximations and exact exchange with a fixed admixing parameter, six local hybrid functionals where the admixing parameters are extended to be spatially dependent, the SCAN and r 2 SCAN meta-generalized gradient approximations (GGAs), and two widely used GGAs. We found that global hybrids tested in this work have a tendency to over-correct the error in magnetic coupling parameters from the Perdew–Burke–Ernzerhof (PBE) GGA as seen for manganese complexes. The performance of local hybrid density functionals shows no improvement in terms of bias and is scattered without a clear trend, suggesting that more efforts are needed for the extension from global to local hybrid density functionals for this particular property. The SCAN and r 2 SCAN meta-GGAs are found to perform as well as benchmark global hybrids on most tested complexes. We further analyze the charge density redistribution of meta-GGAs as well as global and local hybrid density functionals with respect to that of PBE, in connection to the self-interaction error or delocalization error.

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

Formation energy puzzle in intermetallic alloys: Random phase approximation fails to predict accurate formation energies

We performed density functional calculations to estimate the formation energies of intermetallic alloys. We used two semilocal approximations, the generalized gradient approximation (GGA) by Perdew-Burke- Ernzerhof (PBE) and the strongly constrained and appropriately normed (SCAN) meta-GGA. In addition, we utilized two nonlocal DFT functionals, the hybrid HSE06, and the state-of-the-art random phase approximation (RPA). The nonlocal functionals such as HSE06 and RPA yield accurate formation energies of binary alloys with completely-filled d-band metals, where semilocal functionals underperform. The accuracy at the nonlocal functionals is greatly reduced when a partially-filled d-band metal is present in an alloy, while PBE-GGA outperforms in these cases. We show that the accurate prediction of formation energies by any DFT method depends on its ability to predict the accurate electronic properties, e.g., valence d-band contribution to the density of states (DOS). The SCAN meta-GGA often corrects the PBE-DOS, however, it does not provide accurate formation energies compared to PBE. This is assumed to be due to the lack of proper error cancellation that should be expected due to the similar bulk nature of both alloys and their constituents, which may improve with the modification of meta-GGA ingredients. RPA yields too negative formation energies of alloys with partially-filled d-band metals. RPA results can be corrected by restoring the exchange-correlation kernel, thereby improving the short-range electron-electron correlation in metallic densities.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Re-examining the silicon self-interstitial charge states and defect levels: A density functional theory and bounds analysis study

The self-interstitial atom (SIA) is one of two fundamental point defects in bulk Si. Isolated Si SIAs are extremely difficult to observe experimentally. Even at very low temperatures, they anneal before typical experiments can be performed. Given the challenges associated with experimental characterization, accurate theoretical calculations provide valuable information necessary to elucidate the properties of these defects. Previous studies have applied Kohn–Sham density functional theory (DFT) to the Si SIA, using either the local density approximation or the generalized gradient approximation to the exchange-correlation (XC) energy. The consensus of these studies indicates that a Si SIA may exist in five charge states ranging from -2 to +2 with the defect structure being dependent on the charge state. This study aims to re-examine the existence of these charge states in light of recently derived “approximate bounds” on the defect levels obtained from finite-size supercell calculations and new DFT calculations using both semi-local and hybrid XC approximations. We conclude that only the neutral and +2 charge states are directly supported by DFT as localized charge states of the Si SIA. Within the current accuracy of DFT, our results indicate that the +1 charge state likely consists of an electron in a conduction-band-like state that is coulombically bound to a +2 SIA. Furthermore, the -1 and -2 charge states likely consist of a neutral SIA with one and two additional electrons in the conduction band, respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Bending as a control knob for the electronic and optical properties of phosphorene nanoribbons

We have assessed mechanical bending as a powerful controlling tool for the electronic structure and optical properties of phosphorene nanoribbons. We use state-of-the-art density functional approximations in our work. The overall performance of the recently developed meta-generalized gradient approximation (meta-GGA) mTASK [Phys. Rev. Materials 5, 063803 (2021)] functional establishes the method as a useful alternative to the screened hybrid HSE06 for better band gaps of phosphorene nanoribbons. We present a detailed analysis to interpret the optical absorption of bent phosphorene nanoribbons using the GW-Bethe-Salpeter approximation. Finally, we demonstrate the important role of the unoccupied in-gap state and conclude that this in-gap state in armchair nanoribbons introduced by bending can significantly affect the properties of low-energy excitons and add some useful opportunities for applications in optoelectronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Hydrogen-induced degradation dynamics in silicon heterojunction solar cells via machine learning

Abstract Among silicon-based solar cells, heterojunction cells hold the world efficiency record. However, their market acceptance is hindered by an initial 0.5% per year degradation of their open circuit voltage which doubles the overall cell degradation rate. Here, we study the performance degradation of crystalline-Si/amorphous-Si:H heterojunction stacks. First, we experimentally measure the interface defect density over a year, the primary driver of the degradation. Second, we develop SolDeg, a multiscale, hierarchical simulator to analyze this degradation by combining Machine Learning, Molecular Dynamics, Density Functional Theory, and Nudged Elastic Band methods with analytical modeling. We discover that the chemical potential for mobile hydrogen develops a gradient, forcing the hydrogen to drift from the interface, leaving behind recombination-active defects. We find quantitative correspondence between the calculated and experimentally determined defect generation dynamics. Finally, we propose a reversed Si-density gradient architecture for the amorphous-Si:H layer that promises to reduce the initial open circuit voltage degradation from 0.5% per year to 0.1% per year.

14 SOLAR ENERGY↗
DOE OSTI2022

Electronic structure of strongly correlated systems: recent developments in multiconfiguration pair-density functional theory and multiconfiguration nonclassical-energy functional theory

Strong electron correlation plays an important role in transition-metal and heavy-metal chemistry, magnetic molecules, bond breaking, biradicals, excited states, and many functional materials, but it provides a significant challenge for modern electronic structure theory. The treatment of strongly correlated systems usually requires a multireference method to adequately describe spin densities and near-degeneracy correlation. However, quantitative computation of dynamic correlation with multireference wave functions is often difficult or impractical. Multiconfiguration pair-density functional theory (MC-PDFT) provides a way to blend multiconfiguration wave function theory and density functional theory to quantitatively treat both near-degeneracy correlation and dynamic correlation in strongly correlated systems; it is more affordable than multireference perturbation theory, multireference configuration interaction, or multireference coupled cluster theory and more accurate for many properties than Kohn–Sham density functional theory. This perspective article provides a brief introduction to strongly correlated systems and previously reviewed progress on MC-PDFT followed by a discussion of several recent developments and applications of MC-PDFT and related methods, including localized-active-space MC-PDFT, generalized active-space MC-PDFT, density-matrix-renormalization-group MC-PDFT, hybrid MC-PDFT, multistate MC-PDFT, spin–orbit coupling, analytic gradients, and dipole moments. We also review the more recently introduced multiconfiguration nonclassical-energy functional theory (MC-NEFT), which is like MC-PDFT but allows for other ingredients in the nonclassical-energy functional. We discuss two new kinds of MC-NEFT methods, namely multiconfiguration density coherence functional theory and machine-learned functionals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

How well do self-interaction corrections repair the overestimation of static polarizabilities in density functional calculations?

Herein, we examine the effect of removing self-interaction error (SIE) on the calculation of molecular polarizabilities in the local spin density (LSDA) and generalized gradient approximations (GGA). To this end, we utilize a database of 132 molecules taken from a recent benchmark study [Hait and Head-Gordon, Phys. Chem. Chem. Phys. , 2018, 20 , 19800] to assess the influence of SIE on polarizabilities by comparing results with accurate reference data. Our results confirm that the general overestimation of molecular polarizabilities by these density functional approximations can be attributed to SIE. However, removing SIE using the Perdew–Zunger self-interaction-correction (PZ-SIC) method, implemented using the Fermi–Löwdin Orbital SIC approach, leads to an underestimation of molecular polarizabilities, showing that PZ-SIC overcorrects when combined with LSDA or GGA. Application of a recently proposed locally scaled SIC [Zope, et al., J. Chem. Phys. , 2019, 151 , 214108] is found to provide more accurate polarizabilities. We attribute this to the ability of the local scaling scheme to selectively correct for SIE in the regions of space where the correction is needed most.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Skyrme pseudopotentials at next-to-next-to-leading order: Construction of local densities and first symmetry-breaking calculations

There is an ongoing quest to improve on the spectroscopic quality of nuclear energy density functionals (EDFs) of the Skyrme type through extensions of its traditional form. One direction for such activities is the inclusion of terms of higher order in gradients in the EDF. We report on exploratory symmetry-breaking calculations performed for an extension of the Skyrme EDF that includes central terms with four gradients at next-to-next-to-leading order (N2LO) and for which the high-quality parametrization SN2LO1 has been constructed recently. Up to now, the investigation of such functionals with higher-order terms was limited to infinite matter and spherically symmetric configurations of singly and doubly magic nuclei. We address here nuclei and phenomena that require us to consider axial and nonaxial deformation, both for reflection-symmetric and also reflection-asymmetric shapes, as well as the breaking of time-reversal invariance. Achieving these calculations demanded a number of formal developments. These all resulted from the formulation of the N2LO EDF requiring the introduction of new local densities with additional gradients that are not present in the EDF at NLO. Their choice is not unique, but can differ in the way the gradients are coupled. While designing a numerical implementation of N2LO EDFs in Cartesian three-dimensional coordinate-space representation, we have developed a novel definition and a new unifying notation for normal and pair densities that contain gradients at arbitrary order. Besides having mnemonic advantages, the new notation allows for the easy identification of redundancies and reducibilities in a given set of local densities, and the new definition makes it straightforward to construct densities that automatically adopt the symmetries of the many-body state they are constructed from. The resulting scheme resolves several issues with some of the choices that have been made for local densities in the past, in particular when breaking time-reversal symmetry. Guided by general practical considerations, we propose an alternative form of the N2LO contribution to the Skyrme EDF that is built from a different set of densities. It has exactly the same physics content, but is much more efficient to handle in formal discussions and, compared to the original formulation, leads to a substantial reduction of computational cost and memory requirements in deformed codes. As representative examples for the performance of SN2LO1, we have chosen the ground states of even-even Kr and Nd isotopes, the fission barrier of 240 Pu as well as the superdeformed rotational band of 194 Hg. Overall, for the nuclei and phenomena studied here, the SN2LO1 parametrization does not yet present a systematic improvement over standard NLO parametrizations. This finding calls for improved fit protocols that better discriminate between NLO and N2LO terms and better exploit the unique features of the additional degrees of freedom offered by the latter.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗