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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 NTRS1990

Universal energy relations and metal/ceramic interfaces

Known general relationships between pertinent variables are applied to investigate metal-ceramic interfaces. The adhesive energy is determined. The electronic exchange-correlation energy is found to be the dominant attractive term in the total energy. Results for the adhesive energy are obtained for junctions of all combinations of the low index surfaces of Al,Na, Mg, and Zn. This leads to a variety of curves, all with a single minimum of separation and equilibrium binding energy. Scaling results for 10 contacts fall closely onto a single curve, a universal energy relation for adhesion. The scaled chemisorption curves fall accurately on the same universal form that was found for adhesion. For the case of cohesion, all-first principle results are scaled and again all scaled curves for a variety of metals fall accurately on the universal form for adhesion and chemisorption. An intimate relationship between the energetics of solids and molecules is inferred.

Smith, John R.↗
DOE OSTI2020

Finite-temperature coupled cluster: Efficient implementation and application to prototypical systems

In this work, we discuss the theory and implementation of the finite temperature coupled cluster singles and doubles (FT-CCSD) method including the equations necessary for an efficient implementation of response properties. Numerical aspects of the method including the truncation of the orbital space and integration of the amplitude equations are tested on some simple systems, and we provide some guidelines for applying the method in practice. The method is then applied to the 1D Hubbard model, the uniform electron gas (UEG) at warm, dense conditions, and some simple materials. The performance of model systems at high temperatures is encouraging: for the one-dimensional Hubbard model, FT-CCSD provides a qualitatively accurate description of finite-temperature correlation effects even at U = 8, and it allows for the computation of systematically improvable exchange–correlation energies of the warm, dense UEG over a wide range of conditions. We highlight the obstacles that remain in using the method for realistic ab initio calculations on materials

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Cross-correlation of Dark Energy Survey Year 3 lensing data with ACT and P l a n c k thermal Sunyaev-Zel’dovich effect observations. II. Modeling and constraints on halo pressure profiles

Hot, ionized gas leaves an imprint on the cosmic microwave background via the thermal Sunyaev-Zel’dovich (tSZ) effect. The cross-correlation of gravitational lensing (which traces the projected mass) with the tSZ effect (which traces the projected gas pressure) is a powerful probe of the thermal state of ionized baryons throughout the Universe and is sensitive to effects such as baryonic feedback. In a companion paper (Gatti et al. Phys. Rev. D 105, 123525 (2022)), we present tomographic measurements and validation tests of the cross-correlation between Galaxy shear measurements from the first three years of observations of the Dark Energy Survey and tSZ measurements from a combination of Atacama Cosmology Telescope and Planck observations. In this work, we use the same measurements to constrain models for the pressure profiles of halos across a wide range of halo mass and redshift. We find evidence for reduced pressure in low-mass halos, consistent with predictions for the effects of feedback from active Galactic nuclei. We infer the hydrostatic mass bias (B ≡ M 500c /M SZ from our measurements, finding B = 1.8 ± 0.1 when adopting the Planck-preferred cosmological parameters. We additionally find that our measurements are consistent with a nonzero redshift evolution of B, with the correct sign and sufficient magnitude to explain the mass bias necessary to reconcile cluster count measurements with the Planck-preferred cosmology. Our analysis introduces a model for the impact of intrinsic alignments (IAs) of galaxy shapes on the shear-tSZ correlation. We show that IA can have a significant impact on these correlations at current noise levels.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Connected three-body terms in single-reference unitary many-body theories: Iterative and perturbative approximations

This work introduces various approaches to include connected three-body terms in unitary many-body theories, focusing on the driven similarity renormalization group (DSRG). Starting from the least approximate method—the linearized DSRG truncated to one-, two-, and three-body operators [LDSRG(3)]—we develop several approximate LDSRG(3) models with reduced computational cost. Through a perturbative analysis, we motivate a family of iterative LDSRG(3)-n and -n' (n = 1, 2, 3, 4) methods that contain a subset of the LDSRG(3) diagrams. Among these variants, the LDSRG(3)-2 scheme has the same computational complexity of coupled cluster theory with singles, doubles, and triples (CCSDT), but it outperforms CCSDT in the accuracy of the predicted correlation energies. We also propose and implement two perturbative triples corrections based on the linearized DSRG truncated to one- and two-body operators augmented with recursive semi-quadratic commutators [qDSRG(2)]. Overall, the resulting qDSRG(2)+(T) approach matches the accuracy of the “gold-standard” coupled cluster theory with singles, doubles, and perturbative triples model on the energetics of twenty-eight closed-shell atoms and small molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

ν-point energy correletors with F AST EEC: Small-x physics from LHC jets

In recent years, energy correlators have emerged as a powerful tool for studying jet substructure, with promising applications such as probing the hadronization transition, analyzing the quark-gluon plasma, and improving the precision of top quark mass measurements. The projected N-point correlator measures correlations between N final-state particles by tracking the largest separation between them, showing a scaling behavior related to DGLAP splitting functions. These correlators can be analytically continued in N, commonly referred to as ν-correlators, allowing access to non-integer moments of the splitting functions. Of particular interest is the ν → 0 limit, where the small momentum fraction behavior of the splitting functions requires resummation. Originally, the computational complexity of evaluating ν-correlators for M particles scaled as 2 2M , making it impractical for real-world analyses. However, by using recursion, we reduce this to M 2M , and through the FastEEC method of dynamically resolving subjets, M is replaced by the number of subjets. This breakthrough enables, for the first time, the computation of ν-correlators for LHC data. In practice, limiting the number of subjets to 16 is sufficient to achieve percent-level precision, which we validate using known integer-ν results and convergence tests for non-integer ν. We have implemented this in an update to FastEEC and conducted an initial study of power-law scaling in the perturbative regime as a function of ν, using CMS Open Data on jets. The results agree with DGLAP evolution, except at small ν, where the anomalous dimension saturates to a value that matches the BFKL anomalous dimension.

Energy correlators↗
DOE OSTI2025

CpFe(CO) 2 Radical Generated from Dinuclear [CpFe(CO) 2 ] 2 and Mononuclear (Cp)(CO) 2 Fe(H): Density Functional Theory Is Accurate for One, But Not Both

Density functional theory (DFT) methods remain the most practical approach to calculating properties and reaction mechanisms of transition metal complexes. While the accuracy of DFT methods has been evaluated for some properties of mononuclear organometallic complexes there has been a general lack of evaluation for dinuclear organometallic complexes, in particular bonding changes related to reaction mechanisms. Here, this work evaluated DFT and coupled cluster methods for the accuracy of calculating the CpFe(CO) 2 radical (Fp•) generated from dinuclear [CpFe(CO) 2 ] 2 (Fp 2 ) and mononuclear [(Cp)(CO) 2 Fe(H)] (Fp-H). This transition metal radical fragment was evaluated because dinuclear complexes built with it have recently shown a variety of unique reactions but has proven challenging to accurately calculate with DFT methods. Here we show that DFT methods provide a surprising wide range of fragmentation energies for Fp 2 and lower and mid rung DFT methods as well as DLPNO–CCSD(T) perform well for this dissociation energy. The highest rung double-hybrid methods have a large range in the Fp 2 dissociation energy, and the energy greatly depends on the amount of MP2 correlation energy included. For generating Fp• from Fp-H the lower and mid rung methods that worked well for Fp 2 showed significant error. Double-hybrid methods unfortunately are only accurate for the Fe–H bond if they are very inaccurate for the Fp 2 dissociation energy. While DLPNO–CCSD(T) is not perfect, and not close to chemically accurate for the Fe–H bond, it does provide reasonable accuracy for both Fp 2 and Fp-H dissociation energies.

density functional theory↗
DOE OSTI2025

Learning local and semi-local density functionals from exact exchange-correlation potentials and energies

Finding accurate exchange-correlation (XC) functionals remains the defining challenge in density functional theory (DFT). Despite 40 years of active development, attaining general purpose chemical accuracy is still elusive with existing functionals. We present a data-driven pathway to learn the XC functional by using the exact density, XC energy, and XC potential. While the exact densities are obtained from accurate configuration interaction (CI), the exact XC energies and XC potentials are obtained via inverse DFT calculations on the CI densities. We demonstrate how simple neural network (NN)–based local density approximation (LDA) and generalized gradient approximation (GGA), trained on just five atoms and two molecules, provide remarkable improvement in total energies and densities. Particularly, the NN-based GGA functional attains similar accuracy as the higher rung SCAN meta-GGA on various thermochemistry datasets. These results underscore the promise of using the XC potential in modeling XC functionals and can pave the way for systematic learning of increasingly accurate XC functionals.

Science & Technology - Other Topics↗
DOE OSTI2026

Optimization of Random Phase Approximation Calculations for Improved Energies of Molecules, Solids, and Surfaces

We present an optimized random phase approximation method (optRPA26) that significantly improves upon conventional RPA through an optimized choice of reference orbitals and energy components, rather than a modification of the RPA correlation functional itself. The method employs an empirically constructed hybrid functional to generate DFT orbitals to evaluate the RPA correlation energy, which is then scaled by a constant. Comprehensive benchmarks across molecules, bulk solids, and surface systems demonstrate that optRPA26 consistently achieves high accuracy, with mean absolute errors of 0.05 eV for W4-11-RE reaction energies, 0.07 eV for cohesive energies, 0.09 eV for metal oxide formation energies, 0.11–0.12 eV for adsorption of small molecules on metals, and 0.06 eV for adsorption on oxides. In addition, optRPA26 correctly captures phase stability in metal oxides and magnetic metals. The optRPA26 approach can be run using standard RPA implementations, highlighting its potential as a general-purpose reference method that can accurately capture covalent, ionic, metallic, and van der Waals bonding in molecules, solids, and interfaces.

Adsorption↗
NASA NTRS2002

Glennan Microsystems Initiative

During the 2001-2002 award period, we performed research on Pt/Ti/bare 6H-SiC and bare 4H-SiC interfaces in order to identify their electronic properties as a function of surface preparation. The overall aim of this work is to optimize the electronic properties of metal contacts to SiC as well as the active SiC material itself as a function of surface preparation and subsequent processing. Initially, this work has involved identifying bare surface, subsurface, and metal induced gap states at the metal-SiC contact and correlating energies and densities of deep levels with Schottky barrier heights. We used low energy electron-excited nanoluminescence (LEEN) spectroscopy, X-ray photoemission spectroscopy (XPS), and Secondary Ion Mass Spectrometry (SIMS) in order to correlate electronic states and energy bands with chemical composition, bonding, and crystal structure. A major development has been the discovery of polytype transformations that occur in 4H-SiC under standard microelectronic process conditions used to fabricate SiC devices. Our results are consistent with the stacking fault generation, defect formation, and consequent degradation of SiC recently reported for state-of-the-art ABB commercial diodes under localized electrical stress. Our results highlight the importance of -optimizing process conditions and material properties - anneal times, temperatures and doping to control such structural changes within epitaxial SiC layers. Thus far, we have established threshold times and temperatures beyond which 4H-SiC exhibits 3C-SiC transformation bands for a subset of dopant concentrations and process conditions. On the basis of this temperature time behavior, we have been able to establish an activation energy of approximately 2.5 eV for polytype transformation and dislocation motion. Work continues to establish the fundamental mechanisms underlying the polytype changes and its dependence on material parameters.

Brillson, Leonard J.↗
DOE OSTI2020

Neutron-Neutron Correlations in the Photofission of 238U

Background: In the fission of actinides, the nearly back-to-back motion of the fission fragments has a strong effect on the kinematics of fission neutrons. This leads to a favoring of opening angles near 0? and 180? in the neutron-neutron (n-n) opening angle distributions of correlated neutron pairs from the same fission event. Purpose: To measure the n-n opening angle and energy correlations in the photofission of 238U. As of this writing, measurements of correlated n-n opening angle distributions have been reported only for the spontaneous and neutron-induced fission of actinides. This work is the first to report such a measurement using photofission and will provide useful experimental input for photofission models used in codes such as MCNP and FREYA. Method: Fission is induced using bremsstrahlung photons produced via a low duty factor, pulsed, linear electron accelerator. The bremsstrahlung photon beam impinges upon a 238U target that is surrounded by a large neutron scintillation detection system capable of measuring particle position and time of flight, from which n-n opening angle and energy are measured. Neutron-neutron angular correlations are determined by taking the ratio between a correlated neutron distribution and an uncorrelated neutron distribution formed by the pairing of neutrons produced during different beam pulses. This analysis technique greatly diminishes effects due to detector efficiencies, acceptance, and experimental drifts. Results: The angular correlation of neutrons from the photofission of 238U shows a high dependence on neutron energy as well as a dependence on the angle of the emitted neutrons with respect to the incoming photon beam. Angular correlations were also measured using neutrons from the spontaneous fission of 252Cf, showing good agreement with past measurements. Conclusions: The measured angular correlations reflect the underlying back-to-back nature of the fission fragments. An anomalous decline in n-n yield was observed for opening angles near 180? for 238U.

Burggraf, Jeff↗
DOE OSTI2023

X-ray Parametric Down Conversion at the APS Synchrotron

We present measurements of X-ray Parametric Down Conversion at the Advanced Photon Source synchrotron facility. We use an incoming pump beam at 22 keV to observe the simultaneous, elastic emission of down-converted photon pairs generated in a diamond crystal. The pairs are detected using high count rate silicon drift detectors with low noise. Production by down-conversion is confirmed by measuring time-energy correlations in the detector signal, where photon pairs within an energy window ranging from 10 to 12 keV are only observed at short time differences. By systematically varying the crystal misalignment and detector positions, we obtain results that are consistent with the constant total of the down-converted signal.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1988

Correlation mass method for analysis of neutrinos from supernova 1987A

Application of a time-energy correlation method to the Kamiokande II (KII) observations of neutrinos apparently emitted from supernova 1987A has yielded a neutrino rest mass of 3.6 eV. A Monte Carlo analysis shows a reconfirming probabilty distribution for the neutrino rest mass peaked at 2.8, and dropping to 50 percent of the peak at 1.4 and 4.8 eV. Although the KII data indicate a very short time scale of emission, over an extended period on the order of 10 sec, both data from the Irvine-Michigan-Brookhaven experiment and the KII data show a tendency for the more energetic neutrinos to be emitted earlier at the source, suggesting the possibility of cooling.

Chiu, Hong-Yee↗
NASA NTRS1967

Estimate of the Total Energy of the Beh(sub 2) Molecule

The existence of gaseous BeH 2 , predicted from simple valence theory, has still not been established experimentally. We have estimated the total energy of this molecule, assumed linear symmetric, as the sum of four negative terms; the calculated SCF energy, the SCF error to the Hartree-Fock limit, the correlation energy to the exact nonrelativistic energy, and the relativistic energy.

Molecular energy↗
NASA NTRS1993

An analysis of isothermal, bithermal, and thermomechanical fatigue data of Haynes 188 and B1900+Hf by energy considerations

The low-cycle fatigue behavior of Haynes 188 and B1900+Hf under isothermal, bithermal, and thermomechanical loading conditions has been analyzed on the basis of the total hysteresis energy expended per cycle. It has been observed that in the case of isothermal fatigue the total hysteresis energy correlates well with the fatigue life. In the case of bithermal 'high rate' fatigue, for a given total hysteresis energy per cycle, the fatigue life is equal to or greater than the isothermal fatigue life at the maximum bithermal temperature. This observation could be used to establish a lower bound on life for design purposes. In one case of bithermal creep-fatigue and in thermomechanical fatigue, the life is shorter than that corresponding to the isothermal life at the maximum temperature. The energy supplied, per se, may not always give a systematic correlation with the fatigue life in the cases where time-dependent creep and environmental effects are encountered. Thus, in bithermal creep-fatigue and thermomechanical fatigue, the role of creep and environment and their dependence on the energy supplied have to be properly accounted for before the energy term can be used for life prediction.

Radhakrishnan, V. M.↗
DOE OSTI2025

Qubit-Efficient Quantum Chemistry with the ADAPT Variational Quantum Eigensolver and Double Unitary Downfolding

Here, in this work, we combine the recently developed double unitary coupled cluster (DUCC) theory with the adaptive, problem-tailored variational quantum eigensolver (ADAPT-VQE) to explore the accuracy of unitary downfolded Hamiltonians for quantum simulation of chemistry. We benchmark the ability of DUCC effective Hamiltonians to recover dynamical correlation energy outside of an active space. We consider the effects of strong correlation, commutator truncation, higher-body terms, and approximate external amplitudes on the accuracy of these effective Hamiltonians. When combining these DUCC Hamiltonians with ADAPT-VQE, we observe similar convergence of the ground state as compared with bare active space Hamiltonians, demonstrating that DUCC Hamiltonians provide increased accuracy without increasing the load on the quantum processor.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1969

Self-consistent many-electron theory of electron work functions and surface potential characteristics for selected metals

Electron work functions, surface potentials, and electron number density distributions and electric fields in the surface region of 26 metals were calculated from first principles within the free electron model. Calculation proceeded from an expression of the total energy as a functional of the electron number density, including exchange and correlation energies, as well as a first inhomogeneity term. The self-consistent solution was obtained via a variational procedure. Surface barriers were due principally to many-body effects; dipole barriers were small only for some alkali metals, becoming quite large for the transition metals. Surface energies were inadequately described by this model, which neglects atomistic effects. Reasonable results were obtained for electron work functions and surface potential characteristics, maximum electron densities varying by a factor of over 60.

Smith, J. R.↗
DOE OSTI2021

Revealing the nature of electron correlation in transition metal complexes with symmetry breaking and chemical intuition

Here, in this work, we provide a nuanced view of electron correlation in the context of transition metal complexes, reconciling computational characterization via spin and spatial symmetry breaking in single-reference methods with qualitative concepts from ligand-field and molecular orbital theories. These insights provide the tools to reliably diagnose the multi-reference character, and our analysis reveals that while strong (i.e., static) correlation can be found in linear molecules (e.g., diatomics) and weakly bound and antiferromagnetically coupled (monometal-noninnocent ligand or multi-metal) complexes, it is rarely found in the ground-states of mono-transition-metal complexes. This leads to a picture of static correlation that is no more complex for transition metals than it is, e.g., for organic biradicaloids. In contrast, the ability of organometallic species to form more complex interactions, involving both ligand-to-metal σ-donation and metal-to-ligand π-backdonation, places a larger burden on a theory's treatment of dynamic correlation. We hypothesize that chemical bonds in which inter-electron pair correlation is non-negligible cannot be adequately described by theories using MP2 correlation energies and indeed find large errors vs experiment for carbonyl-dissociation energies from double-hybrid density functionals. A theory's description of dynamic correlation (and to a less important extent, delocalization error), which affects relative spin-state energetics and thus spin symmetry breaking, is found to govern the efficacy of its use to diagnose static correlation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Prototype reactor-antineutrino detector based on 6 Li-doped pulse-shape-discriminating plastic scintillator

An aboveground 60-kg reactor-antineutrino detector prototype, comprising a two-dimensional array of 36 6 ⁢Li-doped pulse-shape-sensitive plastic scintillator bars, is described. Each bar is 50 cm long with a square cross section of 5.5 cm. Doped with 6 ⁢Li at 0.1% by mass, the detector is capable of identifying correlated energy depositions for the detection of reactor antineutrinos via the inverse-𝛽-decay (IDB) reaction. Each bar is wrapped with a specular reflector that directs photons toward photomultiplier tubes mounted at both ends of the bar. Here, this paper highlights the construction, key features, and main performance characteristics of the system. The system, which relies on multiple observables such as pulse-shape discrimination, energy, position, and timing, is capable of detecting IBD-like neutron-correlated backgrounds, long-lived decay chains, and cosmogenic isotopes.

Physics↗