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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 1,459 records · Page 81
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Time-domain theory of transient heat conduction in the local limit

Ultrafast and nanoscale heat conduction demands a unified theoretical framework that rigorously bridges macroscopic transport equations with microscopic material properties derived from statistical physics. Existing empirical generalizations of Fourier's law often lack a solid microscopic foundation, failing to connect observed non-Fourier behavior with underlying atomic-scale mechanisms. In this work, we present a time-domain theory of transient heat conduction rooted in Zwanzig's statistical theory of irreversible processes. Central to this framework is the time-domain transport function $\overleftrightarrow{𝑍}$⁡(𝑡) defined through equilibrium time-correlation functions of heat fluxes. This function generalizes the conventional concept of steady-state thermal conductivity, governing the transition of conduction dynamics from onset second sound type wave propagation at finite speeds to diffusion-dominated behavior across broad temporal and spatial scales. Unlike phonon hydrodynamic models that rely on mesoscopic constructs such as phonon drift velocity, our approach provides a quantitative and microscopic description of intrinsic memory effects in transient heat fluxes and applies universally to bulk materials at any temperature or length scale. By integrating atomistic-scale first-principles calculations with continuum-level macroscopic equations, this framework offers a robust foundation for numerical simulations of transient temperature fields. Furthermore, it facilitates the interpretation and design of transient thermal grating experiments using nanometer-scale heat sources and ultrafast laser systems in the extreme ultraviolet and x-ray wavelength ranges, advancing our understanding of heat dissipation dynamics.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2024

GDB-9-Ex_TD-DFT-PBE0: Dataset containing Time Dependent Density Functional Theory (TDDFT) calculations for organic molecules of the GDB-9-Ex dataset.

This dataset contains data-intensive quantum chemical electronic structure calculations for 96,766 organic molecules of the GDB-9-Ex dataset. Calculations were performed using the Time Dependent Density Functional Theory (TDDFT) first principles method using the ORCA software. It provides UV-vis spectra calculations of molecules with a high level of accuracy. The optical spectra behavior was collected based on the optimized molecular geometries in the DFTB method with 3ob parameters. All calculations utilized the def2-TZVP basis sets with the auxiliary def2/J and def2-TZVP/C basis sets. The time-dependent density-functional theory (TDDFT) approach with the PBE0 exchange-correlation functional and ORCAs default integration grid was employed. For the excitation energy calculations, the lowest 50 excitation states were calculated.

AI dataset↗
DOE OSTI2016

The QTP family of consistent functionals and potentials in Kohn-Sham density functional theory

This manuscript presents the second, consistent density functional in the QTP (Quantum Theory Project) family, that is, the CAM-QTP(01). It is a new range-separated exchange-correlation functional in which the non-local exchange contribution is 100% at large separation. It follows the same basic principles of this family that the Kohn-Sham eigenvalues of the occupied orbitals approximately equal the vertical ionization energies, which is not fulfilled by most of the traditional density functional methods. This new CAM-QTP(01) functional significantly improves the accuracy of the vertical excitation energies especially for the Rydberg states in the test set. It also reproduces many other properties such as geometries, reaction barrier heights, and atomization energies.

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

Ground state wave functions for single-band Hubbard models from the Gutzwiller conjugate gradient minimisation theory

The Gutzwiller conjugate gradient minimisation (GCGM) theory is an ab initio quantum many-body theory for computing the ground-state properties of infinite systems. Previous applications of GCGM provides satisfying accuracy of ground-state energy of Hubbard models. In the current work, we address the problem of whether the obtained wave function is a good approximation for the true ground state by comparing the correlation functions with the benchmark data. Additionally, our results confirms the accuracy of the reproduced ground state of the regular Hubbard model, but with some exception for the frustrated Hubbard model.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

A first principles study of the mechanical, electronic, and vibrational properties of lead oxide

The first principles study of the crystal structure, chemical bonds, elastic and mechanical properties, electron energy band structure and density, and normal long-wave vibrations of nine phases of lead monoxide, dioxide, and tetraoxide has been performed under normal and external pressure within the framework of density functional theory (DFT) with the Perdew–Becke–Ernzerhof (PBE) gradient exchange-correlation functional and its hybrid version with a 25-% Hartree–Fock (HF) exchange contribution in the basis of localized atom orbitals. The behavior of physical parameters has been studied using the cold four- and threeparameter equations of state. The parameters of the crystal structures are in satisfactory agreement with experimental data, and elastic constants indicate their mechanical stability and anisotropy in the elastic properties. The elasticity, shear, and Young moduli, hardness, acoustic velocities, and Debye temperature of dioxide on the one hand and monoxide and tetraoxide on the other hand appreciably differ from each other. The difference between electron properties may be explained by the character of hybridization in the upper filled and lower empty energy bands as evident from the density of states. In monoxide, the indirect band gap width decreases with increasing pressure at a rate of 0.16 eV/GPa, and the direct band gap width increases at a rate of 0.13 eV/GPa. To identify crystalline phases, the frequencies and intensities of long-wave modes active in IR and Raman spectra have been calculated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1992

The distribution of galaxies within the 'Great Wall'

The galaxy distribution within the 'Great Wall', the most striking feature in the first three 'slices' of the CfA redshift survey extension is examined. The Great Wall is extracted from the sample and is analyzed by counting galaxies in cells. The 'local' two-point correlation function within the Great Wall is computed and the local correlation length, is estimated 15/h Mpc, about 3 times larger than the correlation length for the entire sample. The redshift distribution of galaxies in the pencil-beam survey by Broadhurst et al. (1990) shows peaks separated about by large 'voids', at least to a redshift of about 0.3. The peaks might represent the intersections of their about 5/h Mpc pencil beams with structures similar to the Great Wall. Under this hypothesis, sampling of the Great Walls shows that l approximately 12/h Mpc is the minimum projected beam size required to detect all the 'walls' at redshifts between the peak of the selection function and the effective depth of the survey.

Ramella, Massimo↗
DOE OSTI2016

Self-consistent implementation of meta-GGA functionals for the ONETEP linear-scaling electronic structure package

Accurate and computationally efficient exchange-correlation functionals are critical to the successful application of linear-scaling density functional theory (DFT). Local and semi-local functionals of the density are naturally compatible with linear-scaling approaches, having a general form which assumes the locality of electronic interactions and which can be efficiently evaluated by numerical quadrature. Presently, the most sophisticated and flexible semi-local functionals are members of the meta-generalized-gradient approximation (meta-GGA) family, and depend upon the kinetic energy density, τ, in addition to the charge density and its gradient. In order to extend the theoretical and computational advantages of τ-dependent meta-GGA functionals to large-scale DFT calculations on thousands of atoms, we have implemented support for τ-dependent meta-GGA functionals in the ONETEP program. In this paper we lay out the theoretical innovations necessary to implement τ-dependent meta-GGA functionals within ONETEP's linear-scaling formalism. We present expressions for the gradient of the τ-dependent exchange-correlation energy, necessary for direct energy minimization. We also derive the forms of the τ-dependent exchange-correlation potential and kinetic energy density in terms of the strictly localized, self-consistently optimized orbitals used by ONETEP. To validate the numerical accuracy of our self-consistent meta-GGA implementation, we performed calculations using the B97M-V and PKZB meta-GGAs on a variety of small molecules. Using only a minimal basis set of self-consistently optimized local orbitals, we obtain energies in excellent agreement with large basis set calculations performed using other codes. Lastly, to establish the linear-scaling computational cost and applicability of our approach to large-scale calculations, we present the outcome of self-consistent meta-GGA calculations on amyloid fibrils of increasing size, up to tens of thousands of atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Combining Theory and Experiment for Multitechnique Characterization of Activated CO 2 on Transition Metal Carbide (001) Surfaces

Early transition metal carbides (TMC; TM = Ti, Zr, Hf, V, Nb, Ta, Mo) with face-centered cubic crystallographic structure have emerged as promising materials for CO 2 capture and activation. Density functional theory (DFT) calculations using the Perdew–Burke–Ernzerhof exchange–correlation functional evidence charge transfer from the TMC surface to CO 2 on the two possible adsorption sites, namely, MMC and TopC, and the electronic structure and binding strength differences are discussed. Further, the suitability of multiple experimental techniques with respect to (1) adsorbed CO2 recognition and (2) MMC/TopC adsorption distinction is assessed from extensive DFT simulations. Results show that ultraviolet photoemission spectroscopies (UPS), work function changes, core level X-ray photoemission spectroscopy (XPS), and changes in linear optical properties could well allow for adsorbed CO2 detection. Only infrared (IR) spectra and scanning tunnelling microscopy (STM) seem to additionally allow for MMC/TopC adsorption site distinction. These findings are confirmed with experimental XPS measurements, demonstrating CO 2 binding on single crystal (001) surfaces of TiC, ZrC, and VC. The experiments also help resolving ambiguities for VC, where CO 2 activation was unexpected due to low adsorption energy, but could be related to kinetic trapping involving a desorption barrier. With a wealth of data reported and direct experimental evidence provided, this study aims to motivate further basic surface science experiments on an interesting case of CO 2 activating materials, allowing also for a benchmark of employed theoretical models.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Incorporation of Thioacetate Pendants on a Polyalkenamer Enables High Extensibility

This study focuses on functionalizing polycyclooctene (PCOE) with thioacetate groups using thiol–ene click chemistry. The ethylene thioacetate (EVSA) copolymers produced vary in thioacetate incorporation (4–25 mol %) via a controlled semibatch addition technique with AIBN dosing. Copolymers with 4–14 mol % thioacetate are semicrystalline, while those with 20–25 mol % are amorphous. Increased functionalization correlates with decreased crystallinity and increased stretchability, with the highest functionalization (25 mol %) showing a modulus of 0.045 MPa and 2000% elongation at break. Here, this behavior is due to the pseudoprecise functionalization of the thioacetate pendants and intrinsic cross-linking that occurs during melt processing. Broadband dielectric spectroscopy (BDS) indicates a low activation energy barrier (16 kJ/mol for the β process), suggesting potential self-healing applications.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Onset of simple liquid behaviour in modified water models

The transition to simple liquid behaviour is studied in a set of modified hybrid water models where the potential energy contribution of the Lennard-Jones dispersion-repulsion contribution is progressively enhanced relative to the electrostatic contribution. Characteristics of simple liquid behaviour that indicate the extent to which a given system can be mapped onto an inverse power law fluid are examined, including configurational energy-virial correlations, functional form of temperature dependence of the excess entropy along isochores, and thermodynamic and excess entropy scaling of diffusivities. As the Lennard-Jones contribution to the potential energy function increases, the strength of the configurational energy-virial correlations increases. The Rosenfeld-Tarazona temperature dependence of the excess entropy is found to hold for the range of state points studied here for all the hybrid models, regardless of the degree of correlating character. Thermodynamic scaling is found to hold for weakly polar fluids with a moderate degree of energy-virial correlations. Rosenfeld-scaling of transport properties is found not to be necessarily linked with the strength of energy-virial correlations but may hold for systems with poor thermodynamic scaling if diffusivities and excess entropies show correlated departures from the isomorph-invariant behaviour characteristic of approximate inverse power law fluids. The state-point dependence of the configurational energy-virial correlation coefficient and the implications for thermodynamic and excess entropy scalings are considered.

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

Hierarchy of model Kohn–Sham potentials for orbital-dependent functionals: A practical alternative to the optimized effective potential method

We describe a method for constructing a hierarchy of model potentials approximating the functional derivative of a given orbital-dependent exchange-correlation functional with respect to electron density. Each model is derived by assuming a particular relationship between the self-consistent solutions of Kohn–Sham (KS) and generalized Kohn–Sham (GKS) equations for the same functional. In the KS scheme, the functional is differentiated with respect to density, in the GKS scheme—with respect to orbitals. The lowest-level approximation is the orbital-averaged effective potential (OAEP) built with the GKS orbitals. The second-level approximation, termed the orbital-consistent effective potential (OCEP), is based on the assumption that the KS and GKS orbitals are the same. It has the form of the OAEP plus a correction term. The highest-level approximation is the density-consistent effective potential (DCEP), derived under the assumption that the KS and GKS electron densities are equal. The analytic expression for a DCEP is the OCEP formula augmented with kinetic-energy-density-dependent terms. In the case of exact-exchange functional, the OAEP is the Slater potential, the OCEP is roughly equivalent to the localized Hartree–Fock approximation and related models, and the DCEP is practically indistinguishable from the true optimized effective potential for exact exchange. All three levels of the proposed hierarchy require solutions of the GKS equations as input and have the same affordable computational cost.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

An assessment of low-lying excitation energies and triplet instabilities of organic molecules with an ab initio Bethe-Salpeter equation approach and the Tamm-Dancoff approximation

The accurate prediction of singlet and triplet excitation energies is an area of intense research of significant fundamental interest and critical for many applications. Most calculations of singlet and triplet energies use time-dependent density functional theory (TDDFT) in conjunction with an approximate exchange-correlation functional. In this work, we examine and critically assess an alternative method for predicting low-lying neutral excitations with similar computational cost, the ab initio Bethe-Salpeter equation (BSE) approach, and compare results against high-accuracy wavefunction-based methods. We consider singlet and triplet excitations of 27 prototypical organic molecules, including members of Thiel’s set, the acene series, and several aromatic hydrocarbons exhibiting charge-transfer-like excitations. Analogous to its impact in TDDFT, we find that the Tamm-Dancoff approximation (TDA) overcomes triplet instabilities in the BSE approach, improving both triplet and singlet energetics relative to higher level theories. Lastly, we find that BSE-TDA calculations built on effective DFT starting points, such as those utilizing optimally tuned range-separated hybrid functionals, can yield accurate singlet and triplet excitation energies for gas-phase organic molecules.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

Measurement of galaxy clustering at z ∼ 7.2 and the evolution of galaxy bias from 3.8 < z < 8 in the XDF, GOODS-S, and GOODS-N

Lyman-break galaxy (LBG) samples observed during reionization (z ≳ 6) with the Hubble Space Telescope's Wide Field Camera 3 are reaching sizes sufficient to characterize their clustering properties. Using a combined catalog from the Hubble eXtreme Deep Field and CANDELS surveys, containing N = 743 LBG candidates at z ≥ 6.5 at a mean redshift of z-bar =7.2, we detect a clear clustering signal in the angular correlation function (ACF) at ≳ 4σ, corresponding to a real-space correlation length r{sub 0}=6.7{sub −1.0}{sup +0.9}h{sup −1}cMpc. The derived galaxy bias b=8.6{sub −1.0}{sup +0.9} is that of dark matter halos of M=10{sup 11.1{sub −}{sub 0}{sub .}{sub 3}{sup +{sup 0{sup .{sup 2}}}}} M{sub ⊙} at z = 7.2, and highlights that galaxies below the current detection limit (M{sub AB} ∼ –17.7) are expected in lower-mass halos (M ∼ 10{sup 8}-10{sup 10.5} M{sub ⊙} ). We compute the ACF of LBGs at z ∼ 3.8 – z ∼ 5.9 in the same surveys. A trend of increasing bias is found from z-bar =3.8 (b ∼ 3.0) to z-bar =7.2 (b ∼ 8.6), broadly consistent with galaxies at fixed luminosity being hosted in dark matter halos of similar mass at 4 ≲ z ≲ 6, followed by a slight rise in halo masses at z ≳ 7 (∼2σ confidence). Separating the data at the median luminosity of the z-bar =7.2 sample (M {sub UV} = –19.4) shows higher clustering at z-bar =5.9 for bright galaxies (r{sub 0}=5.5{sub −1.6}{sup +1.4}h{sup −1}cMpc, b=6.2{sub −1.5}{sup +1.2}) compared to faint galaxies (r{sub 0}=1.9{sub −1.0}{sup +1.1}h{sup −1}cMpc, b=2.7{sub −1.2}{sup +1.2}) implying a constant mass-to-light ratio (dlogM/dlogL)∼1.2{sub −0.8}{sup +1.8}. A similar trend is present in the z-bar =7.2 sample with larger uncertainty. Finally, our bias measurements allow us to investigate the fraction of dark matter halos hosting UV-bright galaxies (the duty cycle, ε{sub DC}). At z-bar =7.2 values near unity are preferred, which may be explained by the shortened halo assembly time at high redshift.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Real-time scattering in Ising field theory using matrix product states

We study scattering in Ising field theory (IFT) using matrix product states and the time-dependent variational principle. IFT is a one-parameter family of strongly coupled nonintegrable quantum field theories in 1+1 dimensions, interpolating between massive free fermion theory and Zamolodchikov's integrable massive 𝐸 8 theory. Particles in IFT may scatter either elastically or inelastically. In the postcollision wave function, particle tracks from all final-state channels occur in superposition; processes of interest can be isolated by projecting the wave function onto definite particle sectors, or by evaluating energy density correlation functions. Using numerical simulations we determine the time delay of elastic scattering and the probability of inelastic particle production as a function of collision energy. We also study the mass and width of the lightest resonance near the 𝐸 8 point in detail. Close to both the free fermion and 𝐸 8 theories, our results for both elastic and inelastic scattering are in good agreement with expectations from form-factor perturbation theory. Using numerical computations to go beyond the regime accessible by perturbation theory, we find that the high-energy behavior of the two-to-two particle scattering probability in IFT is consistent with a conjecture of Zamolodchikov. Our results demonstrate the efficacy of tensor-network methods for simulating the real-time dynamics of strongly coupled quantum field theories in 1+1 dimensions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Rehabilitation of the Perdew-Burke-Ernzerhof generalized gradient approximation for layered materials

The structural and energetic properties of layered materials present a challenge to density functional theory with common semilocal approximations to the exchange-correlation energy. By combining the most widely used semilocal generalized gradient approximation (GGA), the Perdew-Burke-Ernzerhof (PBE) one, with the revised Vydrov–van Voorhis nonlocal correlation functional (rVV10), both excellent structural and energetic properties of 28 layered materials have been recovered with a judicious parameter selection. We term the resulting functional PBE+rVV10L, with the “L” indicating that it is for layered materials. Such a combination is not new, and only involves refitting a single global parameter. However, the resulting high accuracy suggests such a dispersion-corrected PBE for many aspects of theoretical studies on layered materials. For comparison, we also present the results for PBE+rVV10 where the parameter is determined by 22 interaction energies between molecules.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites

Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. Here, this work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.

36 MATERIALS SCIENCE↗
NASA NTRS1989

Ginzburg-Landau theory for the solid-liquid interface of bcc elements. II - Application to the classical one-component plasma, the Wigner crystal, and He-4

The previously developed Ginzburg-Landau theory for calculating the crystal-melt interfacial tension of bcc elements to treat the classical one-component plasma (OCP), the charged fermion system, and the Bose crystal. For the OCP, a direct application of the theory of Shih et al. (1987) yields for the surface tension 0.0012(Z-squared e-squared/a-cubed), where Ze is the ionic charge and a is the radius of the ionic sphere. Bose crystal-melt interface is treated by a quantum extension of the classical density-functional theory, using the Feynman formalism to estimate the relevant correlation functions. The theory is applied to the metastable He-4 solid-superfluid interface at T = 0, with a resulting surface tension of 0.085 erg/sq cm, in reasonable agreement with the value extrapolated from the measured surface tension of the bcc solid in the range 1.46-1.76 K. These results suggest that the density-functional approach is a satisfactory mean-field theory for estimating the equilibrium properties of liquid-solid interfaces, given knowledge of the uniform phases.

Zeng, X. C.↗