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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 613 records · Page 34
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Ab Initio Electron-Phonon Interactions in Correlated Electron Systems

Electron-phonon ( e - ph ) interactions are pervasive in condensed matter, governing phenomena such as transport, superconductivity, charge-density waves, polarons, and metal-insulator transitions. First-principles approaches enable accurate calculations of e - ph interactions in a wide range of solids. However, they remain an open challenge in correlated electron systems (CES), where density functional theory often fails to describe the ground state. Therefore reliable e - ph calculations remain out of reach for many transition metal oxides, high-temperature superconductors, Mott insulators, planetary materials, and multiferroics. Here we show first-principles calculations of e - ph interactions in CES, using the framework of Hubbard-corrected density functional theory ( DFT + U ) and its linear response extension ( DFPT + U ), which can describe the electronic structure and lattice dynamics of many CES. We showcase the accuracy of this approach for a prototypical Mott system, CoO, carrying out a detailed investigation of its e - ph interactions and electron spectral functions. While standard DFPT gives unphysically divergent and short-ranged e - ph interactions, DFPT + U is shown to remove the divergences and properly account for the long-range Fröhlich interaction, allowing us to model polaron effects in a Mott insulator. Our work establishes a broadly applicable and affordable approach for quantitative studies of e - ph interactions in CES, a novel theoretical tool to interpret experiments in this broad class of materials.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Species, Pathways, and Timescales for NH 3 Formation by Low-Temperature Atmospheric Pressure Plasma Catalysis

Species, pathways, and timescales for NH3 production by plasma catalysis over transition-metal wools are determined by measuring plasma-derived species densities [N, H, and N 2 (v)], quantitatively correlating consumption of these species with NH 3 formation, and measuring consumption of plasma-derived species at different residence times. These findings are enabled by a capillary flow through Ar/N 2 /H 2 plasma jet reactor setup that allows for the measurement of gas-phase species densities by molecular beam mass spectrometry. Surface-mediated reactions involving N radicals are responsible for NH 3 formation over Fe, Ni, and Ag surfaces. N reacts to form NH 3 with ~100% selectivity over Ni and Ag when H/N > 3 and % H 2 ≥ 0.5. The selectivity to ammonia drops as H and H 2 densities decrease for each catalyst. A comparison between amounts of NH 3 formed and N consumed with and without catalysts present shows that surface reactions enable higher and more selective conversion of N to NH 3 than gas-phase reactions alone. The conversion of N to NH 3 is negligible in the absence of H, demonstrating that H is required to produce NH 3 at these operating conditions. The consumption of N occurs on the same timescale as NH 3 formation, further confirming that reactions involving N contribute to NH 3 formation. Though vibrationally excited N 2 [N 2 (v)] is produced in quantities exceeding N by 100-fold, consumption of N 2 (v) on the catalytic surface does not contribute to NH 3 formation. Furthermore, these findings show that for low-temperature atmospheric pressure plasma catalysis, surface- mediated reactions among radical N and H species drive NH 3 formation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Accurate Kohn-Sham auxiliary system from the ground-state density of solids

The Kohn-Sham (KS) system is an auxiliary system whose effective potential is unknown in most cases. It is in principle determined by the ground-state density and it has been found numerically for some low-dimensional systems by inverting the KS equations starting from a given accurate density. For solids, only approximate results are available. In this work, we determine accurate exchange-correlation (xc) potentials for Si and NaCl using the ground-state densities obtained from auxiliary field quantum Monte Carlo calculations. We show that these xc potentials can be rationalized as an ensemble of a few local functions of the density, whose form depends on the specific environment and can be well characterized by the gradient of the density and the local kinetic energy density. Further, the KS band structure can be obtained with high accuracy. The true KS band gap turns out to be larger than the prediction of the local density approximation, but significantly smaller than the measurable photoemission gap, which confirms previous estimates. Finally, our findings show that the conjecture that very different xc potentials can lead to very similar densities and other KS observables is true also in solids, which questions the meaning of details of the potentials and, at the same time, confirms the stability of the KS system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Theory of criticality for quantum ferroelectric metals

A variety of compounds, for example, doped paraelectrics and polar metals, exhibit both ferroelectricity and correlated electronic phenomena such as low-density superconductivity and anomalous transport. Characterizing such properties is tied to understanding the quantum dynamics of inversion symmetry breaking in the presence of itinerant electrons. Here, we present a comprehensive analysis of the properties of a metal near a quantum critical transition to a ferroelectric state, in both two and three dimensions. In this study, starting from a minimal model of electrons coupled to a transverse polar phonon via a Rashba-type spin-orbit interaction, we compute the dynamical response of both electrons and phonons. We find that the system can evince both Fermi and non-Fermi liquid phases, as well as enhanced pairing in both singlet and triplet channels. Furthermore, we systematically compute corrections to one-loop theory and find a tendency to quantum order-by-disorder, leading to a phase diagram that can include second-order, first-order, and finite-momentum phase transitions. Finally, we show that the entire phase diagram can be controlled via application of external strain, either compressive or volume-preserving. Our results provide a map of the dynamical and thermodynamical phase space of quantum ferroelectic metals, which can serve in characterizing existing materials and in seeking applications for quantum technologies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Current Density Regulated Atomic to Nanoscale Process on Li Deposition and Solid Electrolyte Interphase Revealed by Cryogenic Transmission Electron Microscopy

Current density has been perceived to play a critical rule for controlling Li deposition morphology and solid electrolyte interphase (SEI). However, the atomic level mechanism of current density on Li deposition and the SEI remains unclear. In this work, based on cryogenic transmission electron microscopy imaging combined with energy dispersive X-ray spectroscopy and electron energy loss spectroscopy electronic structure analyses, we reveal the atomic level correlation of Li deposition morphology and SEI with current density. We discover that increasing current density leads to increased overpotential for Li nucleation and growth, leading to the transition from growth-limited to nucleation-limited mode for Li dendrite. Independence of current density, the electrochemically deposited Li metal (EDLi) exhibits crystalline whisker-like morphology. The SEI formed at low current density (0.1 mA cm -2 ) is monolithic amorphous; while, a current density of above 2 mA cm -2 leads to a mosaic structured SEI, featuring an amorphous matrix with Li 2 O and LiF dispersoids, and the thickness of the SEI increases with the increase of current density. Uniquely, the Li 2 O particles is spatially located at the top surface of the SEI, while LiF is spatially adjacent to the Li-SEI interface. These results highlight the possible tuning of crucial structural and chemical features of EDLi and SEI through altering deposit conditions and consequently direct correlation with electrochemical performance.

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

Huzinaga projection embedding for efficient and accurate energies of systems with localized spin-densities

We demonstrate the accuracy and efficiency of the restricted open-shell and unrestricted formulation of the absolutely localized Huzinaga projection operator embedding method. Restricted open-shell and unrestricted Huzinaga projection embedding in the full system basis is formally exact to restricted open-shell and unrestricted Kohn–Sham density functional theory, respectively. By utilizing the absolutely localized basis, we significantly improve the efficiency of the method while maintaining high accuracy. Furthermore, the absolutely localized basis allows for high accuracy open-shell wave function methods to be embedded into a closed-shell density functional theory environment. The open-shell embedding method is shown to calculate electronic energies of a variety of systems to within 1 kcal/mol accuracy of the full system wave function result. For certain highly localized reactions, such as spin transition energies on transition metals, we find that very few atoms are necessary to include in the wave function region in order to achieve the desired accuracy. This extension further broadens the applicability of our absolutely localized Huzinaga level-shift projection operator method to include open-shell species. Here, we apply our method to several representative examples, such as spin splitting energies, catalysis on transition metals, and radical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Rapidity-dependent spin decomposition of the nucleon

We revisit the two-dimensional Fourier transform of generalized parton distributions (GPDs) at nonzero skewness. At 𝜂 = 0 it reduces to the standard impact-parameter density, while at 𝜂 ≠ 0 it is an off-forward amplitude that we interpret as a genuine parton–nucleon correlation. Its overall strength (the transverse-plane integral of the density) is fixed by the GPD at the kinematic point 𝑡 =−𝑐 𝜂 =−4⁢𝜂 2 ⁢𝑚$^{2}_{𝑁}$/(1 − 𝜂 2 ) and decreases monotonically with the rapidity gap Δ⁢𝑦 = ln⁡[(1+𝜂)/(1−𝜂)] = 2 artanh⁡(𝜂). This rapidity dependence implies rapidity-modified Ji identities that connect helicity, orbital, and total angular momenta of the correlation in closed form. To quantify these effects, we construct leading-twist quark and gluon GPDs in a string-based conformal framework: conformal moments are parametrized by linear open- and closed-string Regge trajectories with slopes constrained by parton distribution functions (PDFs), hadron/glueball spectroscopy, and form-factor data, and GPDs are reconstructed over the full (𝑥,𝜂,𝑡) domain by Mellin-Barnes inversion with next-to-leading order evolution. We find qualitative agreement (and fair quantitative agreement within quoted uncertainties) for several moments and selected nonsinglet 𝑥-space channels at 𝜇 = 2 GeV when compared with lattice QCD, while we also identify channels with visible tension and discuss likely sources (PDF priors and 𝑡-slope systematics).

Gauge-gravity dualities↗
DOE OSTI2025

Welch Method and Bootstrapping Applied to Subcritical Gamma Noise

We measured the prompt neutron decay constant 𝛼 of the CROCUS zero-power reactor at the Swiss Federal Institute of Technology Lausanne using cross-power spectral density (CPSD) analysis of gamma-gamma correlations from two trans-stilbene organic scintillators positioned near the reactor core. We measured critical and subcritical states, with water levels ranging from 960 mm (critical) to 800 mm (𝜌=−1.4 $ subcritical). Our analysis used the Welch method, dividing signal segments for fast Fourier transform (FFT) frequency analysis and applying bootstrapping uncertainty quantification that uses Welch-defined segments. Results demonstrated a clear increase in the measured 𝛼 as reactor reactivity decreased, distinguishing critical from subcritical conditions. At the 960-mm critical level, 𝛼 was estimated at 155.9 ± 0.7 s −1 , and for the 800-mm subcritical level, 𝛼 increased significantly to 367.3 ± 6.9 s –1 . A linear regression of subcritical states yielded a critical estimate of 154.0 ± 3.1 s –1 , aligning with the static 𝛼 estimate at critical. The bootstrapping method produced normally distributed 𝛼 estimates, confirming data consistency. The gamma CPSD 𝛼 estimates clearly distinguish reactor states and improve monitoring of zero-power reactors. The future deployment of modular and microreactors as potential candidates for noise analysis is demonstrated in CROCUS, particularly zero-power mock-ups of new designs. The improvement of noise analysis in the subcritical domain from this work will support experimental data for reactor deployment and procedure.

CROCUS↗
DOE OSTI2020

Quantifying uncertainties and correlations in the nuclear-matter equation of state

We perform statistically rigorous uncertainty quantification (UQ) for chiral effective field theory (χ EFT) applied to infinite nuclear matter up to twice nuclear saturation density. The equation of state (EOS) is based on high-order many-body perturbation theory calculations with nucleon-nucleon and three-nucleon interactions up to fourth order in the χ EFT expansion. From these calculations our newly developed Bayesian machine-learning approach extracts the size and smoothness properties of the correlated EFT truncation error. Furthermore, we then propose a novel extension that uses multitask machine learning to reveal correlations between the EOS at different proton fractions. The inferred in-medium χ EFT breakdown scale in pure neutron matter and symmetric nuclear matter is consistent with that from free-space nucleon-nucleon scattering. These significant advances allow us to provide posterior distributions for the nuclear saturation point and propagate theoretical uncertainties to derived quantities: the pressure and incompressibility of symmetric nuclear matter, the nuclear symmetry energy, and its derivative. Our results, which are validated by statistical diagnostics, demonstrate that an understanding of truncation-error correlations between different densities and different observables is crucial for reliable UQ. The methods developed here are publicly available as annotated Jupyter notebooks.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Implications of PREX-2 on the electric dipole polarizability of neutron-rich nuclei

Background: The recent announcement by the PREX collaboration of an unanticipated thick neutron skin in 208 Pb ($R^{208}_{skin}$) has challenged the understanding of neutron-rich matter in the vicinity of nuclear saturation density. Whereas earlier constraints indicate that the symmetry energy is relatively soft, the PREX-2 result seems to suggest the opposite. Purpose: To confront constraints on the symmetry energy obtained from measurements of the electric dipole polarizability against those informed by the PREX-2 measurement of $R^{208}_{skin}$ and by the correlations that it entails. Methods: Here, covariant energy density functionals informed by the properties of finite nuclei are used to compute the electric dipole response of 48 Ca, 68 Ni, 132 Sn, and 208 Pb. The set of functionals used in this work are consistent with experimental data, yet are flexible enough in that they span a wide range of values of $R^{208}_{skin}$ Results: It is found that theoretical predictions of the electric dipole polarizability that are consistent with the PREX-2 measurement systematically overestimate the corresponding values extracted from the direct measurements of the distribution of electric dipole strength. Conclusions: The neutron skin thickness of 208 Pb extracted from parity violating electron scattering and the electric dipole polarizability measured in photoabsorption experiments are two of the cleanest experimental tools used to constrain the symmetry energy around nuclear saturation density. However, the recent value of $R^{208}_{skin}$ that suggests a fairly stiff symmetry energy stands in stark contrast to the conclusions derived from the electric dipole polarizability. At present, I offer no solution to this dilemma.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

CrI 3 revisited with a many-body ab initio theoretical approach

CrI 3 has recently been shown to exhibit low-dimensional, long-range magnetic ordering from few layers to single layers of CrI 3 . The properties of CrI 3 bulk and few layered systems are uniquely defined by a combination of short-range intralayer and long-range interlayer interactions; including strong correlations, exchange and spin orbit coupling. Unfortunately, both the long-range van der Waals interactions, which are driven by dynamic, many-body electronic correlations and the competing strong intralayer correlations, present a formidable challenging for the local or semi local mean-field approximations employed in workhorse electronic structure approaches like density functional theory. In this work, we employ a sophisticated many-body approach that can simultaneously describe long- and short-range correlations. Herein, we establish that the fixed-node diffusion Monte Carlo (FNDMC) method reproduces the experimental interlayer separation distance of bulk CrI 3 for the high-temperature, monoclinic phase, with a reliable prediction of the interlayer binding energy. We subsequently employed, the FNDMC results to benchmark the accuracy of several density functional theory exchange-correlation approximations.

36 MATERIALS SCIENCE↗
DOE OSTI2024

GradDFT. A software library for machine learning enhanced density functional theory

Density functional theory (DFT) stands as a cornerstone method in computational quantum chemistry and materials science due to its remarkable versatility and scalability. Yet, it suffers from limitations in accuracy, particularly when dealing with strongly correlated systems. To address these shortcomings, recent work has begun to explore how machine learning can expand the capabilities of DFT: an endeavor with many open questions and technical challenges. In this work, we present GradDFT a fully differentiable JAX-based DFT library, enabling quick prototyping and experimentation with machine learning-enhanced exchange–correlation energy functionals. GradDFT employs a pioneering parametrization of exchange–correlation functionals constructed using a weighted sum of energy densities, where the weights are determined using neural networks. Moreover, GradDFT encompasses a comprehensive suite of auxiliary functions, notably featuring a just-in-time compilable and fully differentiable self-consistent iterative procedure. To support training and benchmarking efforts, we additionally compile a curated dataset of experimental dissociation energies of dimers, half of which contain transition metal atoms characterized by strong electronic correlations. The software library is tested against experimental results to study the generalization capabilities of a neural functional across potential energy surfaces and atomic species, as well as the effect of training data noise on the resulting model accuracy.

Chemistry↗
DOE OSTI2020

Observation of Electrically Tunable van Hove Singularities in Twisted Bilayer Graphene from NanoARPES

The possibility of triggering correlated phenomena by placing a singularity of the density of states near the Fermi energy remains an intriguing avenue toward engineering the properties of quantum materials. Twisted bilayer graphene is a key material in this regard because the superlattice produced by the rotated graphene layers introduces a van Hove singularity and flat bands near the Fermi energy that cause the emergence of numerous correlated phases, including superconductivity. Direct demonstration of electrostatic control of the superlattice bands over a wide energy range has, so far, been critically missing. This work examines the effect of electrical doping on the electronic band structure of twisted bilayer graphene using a back-gated device architecture for angle-resolved photoemission measurements with a nano-focused light spot. A twist angle of 12.2° is selected such that the superlattice Brillouin zone is sufficiently large to enable identification of van Hove singularities and flat band segments in momentum space. Finally, the doping dependence of these features is extracted over an energy range of 0.4 eV, expanding the combinations of twist angle and doping where they can be placed at the Fermi energy and thereby induce new correlated electronic phases in twisted bilayer graphene.

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

Orientational Ordering within Semiconducting Polymer Fibrils

Abstract Due to a general paucity of suitable characterization methods, the internal orientational ordering of polymer fibrils has rarely been measured despite its importance particularly for semi‐conducting polymers. An emerging tool with sensitivity to bond orientation is polarized resonant soft X‐ray scattering (P‐RSoXS). Here, P‐RSoXS reveals the molecular arrangement within fibrils (if type I or type II fibrils), the extent of orientation in the fibril crystal, and an explicit crystal‐amorphous interphase. Neat films as well as binary blends with a fullerene derivative are characterized for three different polymers, that are prototypical materials widely used in organic electronics applications. Anisotropic P‐RSoXS patterns reveal two different fibril types. Analysis of the q ‐dependence of the anisotropy from simulated and experimental scattering patterns reveal that neat polymer fibrillar systems likely comprise more than two phases, with the third phase in addition to crystal and amorphous likely being an interphase with distinct density and orientation. Intriguingly, the fibril type correlates to the H‐ or J‐aggregation signature in ultraviolet‐visible (UV–vis) spectroscopy, revealing insight into the fibril formation. Together, the results will open the door to develop more sophisticated structure‐function relationships between chemical design, fibril type, formation pathways and kinetics, interfacial ordering, and eventually device functions.

Mukherjee, Subhrangsu↗
DOE OSTI2021

The Markov gap for geometric reflected entropy

The reflected entropy S R (A : B) of a density matrix ρ AB is a bipartite correlation measure lower-bounded by the quantum mutual information I(A : B). In holographic states satisfying the quantum extremal surface formula, where the reflected entropy is related to the area of the entanglement wedge cross-section, there is often an order-N 2 gap between S R and I. We provide an information-theoretic interpretation of this gap by observing that S R - I is related to the fidelity of a particular Markov recovery problem that is impossible in any state whose entanglement wedge cross-section has a nonempty boundary; for this reason, we call the quantity S R - I the Markov gap. We then prove that for time-symmetric states in pure AdS 3 gravity, the Markov gap is universally lower bounded by log(2)ℓ AdS /2G N times the number of endpoints of the cross-section. We provide evidence that this lower bound continues to hold in the presence of bulk matter, and comment on how it might generalize above three bulk dimensions. Finally, we explore the Markov recovery problem controlling S R - I using fixed area states. This analysis involves deriving a formula for the quantum fidelity — in fact, for all the sandwiched Rényi relative entropies — between fixed area states with one versus two fixed areas, which may be of independent interest. We discuss, throughout the paper, connections to the general theory of multipartite entanglement in holography.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Virtual diffraction simulations using the quasi-coarse-grained dynamics method to understand and interpret plasticity contributions during in situ shock experiments

The dynamic deformation response of metallic materials has contributions from dislocations, deformation twinning, and plastic deformation. The current state-of-art techniques can detail the complex mechanistic history of deformation modes under shock loading in real-time using in situ X-ray diffraction (XRD). However, the capability of these experiments to unravel plasticity contributions is challenging due to limitations in interpreting results and the lack of validation from atomistic simulations. Molecular dynamics (MD) simulations can successfully capture various deformation modes in metals and complement experiments using simulated diffractograms at various stages of evolution. However, the difference in length and time scales of MD simulations and experiments is a substantial obstacle in completing and interpreting in situ diffractograms. Therefore, the existing modeling methods require various approximations to model defect evolution and interaction at the mesoscales. However, while using approximations to correlate the peak broadening behavior to the density of dislocations or the shifts/splitting due to the presence of twins, the interpretations of the plasticity contributions from diffractograms are non-trivial, especially when multiple modes of deformation may be operating. This viewpoint discusses combining a mesoscale modeling method called quasi-coarse-grained dynamics and virtual XRD to characterize the plasticity contributions in BCC metals from slip, twinning, and phase transformation behavior. Furthermore, the combined approach shows promise in bridging the mesoscale gap between the capabilities of atomic-scale simulations and in situ experiments to characterize the dynamic deformation of materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Constructing the Mechanism of Dinoflagellate Luciferin Bioluminescence Using Computation

Dinoflagellate luciferin bioluminescence is unique since it does not rely on decarboxylation but is poorly understood compared to that of firefly, bacteria, and coelenterata luciferins. Here, in this work, we computationally investigate possible protonation states, stereoisomers, a chemical mechanism, and the dynamics of the bioluminescence intermediate that is responsible for chemiexcitation. Using semiempirical dynamics, time-dependent density functional theory static calculations, and a correlation diagram, we find that the intermediate’s functional group that is likely responsible for chemiexcitation is a 4-member ring, a dioxetanol, that undergoes [2π + 2π] cycloreversion and the biolumiphore is the cleaved structure. The simulated emission spectra and luciferase-dependent absorbance spectra agree with the experimental data, giving support to our proposed mechanism and biolumiphore. We also compute circular dichroism spectra of the intermediate’s four stereoisomers to guide future experiments in differentiating them.

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

High Density Two-Component Glasses of Organic Semiconductors Prepared by Physical Vapor Deposition

Physical Vapor Deposition (PVD) is widely utilized for the production of organic semiconductor devices due to its ability to form thin layers with exceptional properties. Although the layers in the device usually consist of two or more components, there is limited understanding about the fundamental characteristics of such multi-component vapor-deposited glasses. Here, spectroscopic ellipsometry was employed to characterize the densities, thermal stabilities and optical properties of co-vapor deposited NPD and TPD glasses across the entire range of composition. We find that co-deposited NPD and TPD form high density glasses with enhanced thermal stability. The dependences of density and stability upon substrate temperature are correlated, and the birefringence of the co-deposited glasses is determined by the reduced substrate temperature of mixtures. Additionally, we observe that the transformation of a highly stable and dense two-component glass into its supercooled liquid initiates from the free surface and propagates into the bulk at constant velocity, like single component PVD glasses. As a result, all these features are consistent with the surface equilibration mechanism.

77 NANOSCIENCE AND NANOTECHNOLOGY↗