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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Spin-selective evolution of the Zhang-Rice state in binary transition metal oxide MnO(001) film

Here, the Zhang-Rice (ZR) state is a strongly hybridized bound state formed by transition-metal and oxygen atoms. The spin fluctuations within the ZR state are known to play an important role in high-T c superconductivity in cuprates. Here, we employ a combination of angle-resolved photoemission spectroscopy (ARPES), x-ray photoemission spectroscopy (XPS), and ab initio embedded dynamical mean-field theory (eDMFT) to investigate the influence of magnetic ordering on the spectral characteristics of the valence band and Mn 2⁢p core-level in MnO (001) ultrathin films. Our results demonstrate that a complex spin-selective evolution of Mn 3⁢d-O2⁢p hybridization develops due to the long-range antiferromagnetic (AFM) ordering. This hybridization significantly alters the spectral shape and weight of the ZR state. Specifically, in the AFM phase, we observed the sharpening of the ZR state and band folding with the periodicity of the AFM unit cell of MnO(001). We also demonstrated a strong connection between the spectral evolution of the ZR state and the non-local screening channels of the photoexcited core holes. Further, our detailed temperature-dependent study reveals the presence of short-range antiferromagnetic correlations that exist at much higher temperatures than Neel temperature (T N ) and shows the evolution of the ZR state across the magnetic transitions and its implication to the core-hole screening in 3⁢d binary transition metal oxides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Spectral-density estimation with the Gaussian integral transform

The spectral-density operator $\hat{ρ}(ω) = δ(ω–\hat{H})$ plays a central role in linear response theory as its expectation value, the dynamical response function, can be used to compute scattering cross sections. In this work, we describe a near optimal quantum algorithm providing an approximation to the spectral density with energy resolution $\Delta$ and error $\epsilon$ using $O(\sqrt{\text{log}_2 (1/ε)[\text{log}_2 (1 / Δ) + \text{log}_2 (1/ε)]/ Δ)}$ operations. This is achieved without using expensive approximations to the time-evolution operator, but instead exploiting qubitization to implement an approximate Gaussian integral transform of the spectral density. Finally, we also describe appropriate error metrics to assess the quality of the spectral function approximations more generally.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Stability of the modulator in a plasma-modulated plasma accelerator

We explore the regime of operation of the modulator stage of a recently proposed laser-plasma accelerator scheme [Phys. Rev. Lett. 127, 184801 (2021)], dubbed the plasma-modulated plasma accelerator (P-MoPA). The P-MoPA scheme offers a potential route to high-repetition-rate, GeV-scale plasma accelerators driven by picosecond-duration laser pulses from, for example, kilohertz thin-disk lasers. The first stage of the P-MoPA scheme is a plasma modulator in which a long, high-energy “drive” pulse is spectrally modulated by copropagating in a plasma channel with the low-amplitude plasma wave driven by a short, low-energy “seed” pulse. The spectrally modulated drive pulse is converted to a train of short pulses, by introducing dispersion, which can resonantly drive a large wakefield in a subsequent accelerator stage with the same on-axis plasma density as the modulator. In this paper we derive the 3D analytic theory for the evolution of the drive pulse in the plasma modulator and show that the spectral modulation is independent of transverse coordinate, which is ideal for compression into a pulse train. We then identify a transverse mode instability (TMI), similar to the TMI observed in optical fiber lasers, which sets limits on the energy of the drive pulse for a given set of laser-plasma parameters. We compare this analytic theory with particle-in-cell (PIC) simulations and find that even higher energy drive pulses can be modulated than those demonstrated in the original proposal.

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

Influence of inhomogeneous stochasticity on the falsifiability of mean-field theories and examples from accretion disc modelling

ABSTRACT Despite spatial and temporal fluctuations in turbulent astrophysical systems, mean-field theories can be used to describe their secular evolution. However, observations taken over time scales much shorter than dynamical time scales capture a system in a single state of its turbulence ensemble. Comparing with mean-field theory can falsify the latter only if the theory is additionally supplied with a quantified precision. The central limit theorem provides appropriate estimates to the precision only when fluctuations contribute linearly to an observable and with constant coherent scales. Here, we introduce an error propagation formula that relaxes both limitations, allowing for non-linear functional forms of observables and inhomogeneous coherent scales and amplitudes of fluctuations. The method is exemplified in the context of accretion disc theories, where inhomogeneous fluctuations in the surface temperature are propagated to the disc emission spectrum – the latter being a non-linear and non-local function of the former. The derived precision depends non-monotonically on emission frequency. Using the same method, we investigate how binned spectral fluctuations in telescope data change with the spectral resolving power. We discuss the broader implications for falsifiability of a mean-field theory.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Thermal modifications of mesons and energy-energy correlators from real-time simulations of a 𝑈⁡(1) lattice gauge theory

We investigate thermal properties of a 𝑈⁡(1) lattice gauge theory in 1 + 1 dimensions through real-time simulations. We extract the spectral functions directly coupling to the pseudoscalar and scalar mesons, demonstrating the thermal modifications of these states with increasing temperatures. Introducing the notion of energy-flow operators, we quantify the temporal buildup of correlations in the energy flows across the lattice. We demonstrate that energy-energy correlators fail to factorize to products of energy flows, both in the vacuum and at nonzero temperature, indicating the presence of nontrivial correlations in the quantum states. Our results constitute a first real-time ab initio study of bound-state thermal broadening and finite temperature energy-flow correlations in a gauge theory, providing a benchmark for future studies of hadronic matter under extreme conditions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Soft X-ray Emission Spectroscopy of Phosphorus Compounds for Energy Conversion and Storage

Phosphorus (P) is a ubiquitous component of materials for energy conversion and storage. Despite the effectiveness of soft X-ray emission spectroscopy (XES) to characterize these complex materials, XES studies of P-containing compounds are still largely missing. In this investigation, the electronic structure and XES signatures from the P L 2,3 -edge are probed for nine solid-state P-containing compounds characterized by various oxidation states and chemical environments: GaP (3−) , InP (3−) , red-P (0) , H 3 P (3+) O 3 , Na 2 H 2 P 2 (4+) O 6 , H 3 P (5+) O 4 , KH 2 P (5+) O 4 , Na 2 HP (5+) O 4 , and InP (5+) O 4 . The XES spectrum of each material exhibits distinct spectral fingerprints, which provide a robust basis for the speciation of complex P-containing samples. Density functional theory calculations shed light on the electronic structure of selected materials and particularly on the effect of phosphorus-oxygen hybridization. This study provides a comprehensive understanding of P L 2,3 XES spectral fingerprints across a wide range of oxidation states and chemical environments. These data sets and insights pave the way for dedicated future work, such as in situ and operando investigations of P-containing compounds in energy-related applications, where speciation of P compounds is needed.

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

Gravitational effective field theory islands, low-spin dominance, and the four-graviton amplitude

Abstract We analyze constraints from perturbative unitarity and crossing on the leading contributions of higher-dimension operators to the four-graviton amplitude in four spacetime dimensions, including constraints that follow from distinct helicity configurations. We focus on the leading-order effect due to exchange by massive degrees of freedom which makes the amplitudes of interest infrared finite. In particular, we place a bound on the coefficient of the R 3 operator that corrects the graviton three-point amplitude in terms of the R 4 coefficient. To test the constraints we obtain nontrivial effective field-theory data by computing and taking the large-mass expansion of the one-loop minimally-coupled four-graviton amplitude with massive particles up to spin 2 circulating in the loop. Remarkably, we observe that the leading EFT coefficients obtained from both string and one-loop field-theory amplitudes lie in small islands. The shape and location of the islands can be derived from the dispersive representation for the Wilson coefficients using crossing and assuming that the lowest-spin spectral densities are the largest. Our analysis suggests that the Wilson coefficients of weakly-coupled gravitational physical theories are much more constrained than indicated by bounds arising from dispersive considerations of 2 → 2 scattering. The one-loop four-graviton amplitudes used to obtain the EFT data are computed using modern amplitude methods, including generalized unitarity, supersymmetric decompositions and the double copy.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Computing nuclear response functions with time-dependent coupled-cluster theory

We compute nuclear response functions by solving the time-dependent 𝐴-body Schrödinger equation, recording the time-dependent transition moment and extracting spectral information via Fourier transforms. The solution of the time-dependent many-body problem accounts for correlations on top of the mean field by taking advantage of a time-dependent formulation of coupled-cluster theory. As a validation, we focus on electric dipole transitions in 4 He and 16 O and compare moments of the response function distribution to the results of an equivalent static framework, finding negligible discrepancies. We investigate how proton and neutron densities evolve in time, and we see the traditional picture of soft and giant dipole resonances as collective oscillations of protons and neutrons emerging from our calculations in 16 O and 24 O. Furthermore, this method also allows us to investigate the behavior of the nucleus in the presence of a strong electric field. In that regime, the behavior of the system becomes chaotic. Qualitatively, the spectral information obtained in this limit is in line with previous time-dependent mean-field results.

Ab initio calculations↗
DOE OSTI2020

Comparing event generator predictions and ab-initio calculations of $\nu$-$^{12}$C neutral current quasi-elastic scattering at 1 GeV

The measurement of neutrino oscillations and exotic physics searches are important parts of the physics program in the near future, with new state-of-the-art experiments planned within the next decade. Future and modern experiments in these fields will make use of nuclear targets. Event Generators (EGs) are software used in the analysis of neutrino oscillation experiments. EGs use to predict kinematic observables for a range of neutrino energies. These simulations may lack physics captured by more rigorous theoretical calculations. This work compares EG performance to nuclear theory calculations by comparing observables generated in the two frameworks. We provide a common set of definitions between theory and experiment and assess the physics contained in EG simulations. Neutral current quasi-elastic (NCQE) scattering events for neutrinos and anti-neutrinos on a $^{12}$C target are simulated with a specific EG, NEUT, used by the T2K experiment for its analysis. The simulated cross sections are compared to analytic calculations from nuclear theory within the factorization scheme. We compare the NEUT implementation of two different models on nuclear spectral functions: the Relativistic Fermi Gas (RFG) and the correlated basis spectral function (CBF) to analytic calculations of the same models in the factorization scheme. For both nuclear physics models, we compare the appearance of features in the distributions relevant to experimental analyses. Qualitatively, the shape of the simulated distribution is similar to the one obtained through theory calculations; however, there are some discrepancies between the theory calculations and the NEUT simulation. While the EG simulations and analytic calculations with the same model of nuclear dynamics show similar overall features, there are still differences between the two.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Efficient Treatment of Large Active Spaces through Multi-GPU Parallel Implementation of Direct Configuration Interaction

In this study, we have extended our graphical processing unit (GPU)-accelerated direct configuration interaction program to multiple devices, reducing iteration times for configuration spaces of 165 million determinants to only 3 s using NVIDIA P100 GPUs. Similar improvements in the one- and two-particle reduced density matrix formation allow for fast analytical energy gradients and electronic properties. Our parallel algorithm enables the calculation of arbitrarily large configuration spaces (limited only by available system memory), with iteration times of 13 min for an active space of 18 electrons in 18 orbitals (2.4 billion determinants) using six consumer grade NVIDIA 1080Ti GPUs. These advances enable routine molecular dynamics simulations, geometry optimizations, and absorption spectrum calculations for molecules with large configuration spaces, a task that has heretofore required massive computational effort. In this work, we demonstrate the utility of our program by generating the absorption spectrum for diphenyl acetylene at the floating occupation molecular orbital complete active space configuration interaction level of theory. Lastly, several active spaces were investigated to assess the dependence of spectral features on orbital space dimension.

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

Deep reinforcement learning for complex evaluation of one-loop diagrams in quantum field theory

In this paper we present a technique based on deep reinforcement learning that allows for numerical analytic continuation of integrals that are often encountered in one-loop diagrams in quantum field theory. To extract certain quantities of two-point functions, such as spectral densities, mass poles or multiparticle thresholds, it is necessary to perform an analytic continuation of the correlator in question. At one-loop level in Euclidean space, this results in the necessity to deform the integration contour of the loop integral in the complex plane of the square of the loop momentum, to avoid nonanalyticities in the integration plane. Using a toy model for which an exact solution is known, we train a reinforcement learning agent to perform the required contour deformations. We report our study shows great promise for an agent to be deployed in iterative numerical approaches used to compute nonperturbative two-point functions, such as the quark propagator Dyson-Schwinger equation, or more generally, Fredholm equations of the second kind, in the complex domain.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Phonon-assisted optical absorption of SiC polytypes from first principles

Silicon carbide (SiC) is an indirect-gap semiconductor material widely used in electronic and optoelectronic applications. While experimental measurements of the phonon-assisted absorption coefficient of SiC across its indirect gap have existed for more than 50 years, theoretical investigations of phonon-assisted absorption have been hampered by their excessive computational cost. Here, in this work, we calculate the phonon-assisted temperature-dependent optical absorption spectra of the commonly occurring SiC polytypes (3C, 2H, 4H, 6H, and 15R), using first-principles approaches based on density functional theory and related techniques. We show that our results agree with experimentally determined absorption coefficients in the spectral region between the direct and indirect band gaps. The temperature dependence of the spectra can be well predicted with taking the temperature dependence of the band gaps into account. Lastly, we compare the spectra obtained with second-order perturbation theory to those determined by the special displacement method and we show that the full consideration of the electronic energy renormalization due to temperature is important to further improve the prediction of the phonon-assisted absorption in SiC. Our insights can be applied to predict the optical spectra of the less common SiC polytypes and other indirect-gap semiconductors in general.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Dynamic control of the spatial frequency content of an intense laser via intra-beam energy transfer

We present theory and simulations demonstrating that bandwidth-inducing optical smoothing techniques such as smoothing by spectral dispersion (SSD) can initiate intra-beam energy transfer (IBET) within a single beam. IBET consists of energy transfer between the different frequency components of the beam and results in a simultaneous and correlated redistribution of the temporal and spatial frequencies of the laser's electric field. We identify a threshold in bandwidth for IBET to occur and validate the theory with simulations. The bandwidth and the color cycling of SSD can result in IBET in conditions relevant for high-energy density experiments at the National Ignition Facility and Omega Laser. We show that IBET could be used to manipulate a laser's spatial frequency content within a plasma. In particular, this technique could be used to increase a laser's effective f-number, with potential applications for self-guiding in plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Measures of illuminant-induced metameric mismatch: theory, comparative analysis, and implications for application

Illuminant-induced metameric mismatch is an important consideration in the specification of light sources for some architectural environments, yet there is currently no standardized performance measure. The goal of this work was to evaluate two recent research proposals: the metameric uncertainty index ( R t ) and the metamer mismatching color rendering index (MMCRI). To compare the relative performance of these two measures, 100,000 spectral power distributions were generated with 3, 4, 5, 6, and 7 Gaussian spectral components and spectral widths varying from 1 nm (monochromatic) to 100 nm. Both measures generally agree with the theory that broadband radiation should cause less metameric mismatch than narrowband radiation. The two measures have relatively better agreement for broadband SPDs and relatively worse agreement for narrower spectra. Despite some similarities, non-parametric statistical tests suggest that R t and MMCRI are significantly different quantifications of illuminant-induced metameric mismatch ( p < 0.0001 for all comparisons). Characteristics of the MMCRI computation that are potentially problematic for applied lighting were observed.

42 ENGINEERING↗
DOE OSTI2021

Hybrid density functional study of band gap engineering of SrTi O 3 photocatalyst via doping for water splitting

Perovskite SrTiO 3 (STO) is an attractive photocatalyst for solar water splitting but suffers from a limited photoresponse in the visible spectral range due to its wide band gap. By means of hybrid density functional theory calculations, we systematically study engineering its band gap via doping 4$\textit{d}$ and 5$\textit{d}$ transition-metals $\textit{M}$ (M = Zr, Nb, Mo, Tc, Ru, Rh, Pd, Hf, Ta, W, Re, Os, Ir, and Pt) and chalcogen elements $\textit{Y}$ ($\textit{Y}$ = S and Se).We find that transition-metal dopant M either has no effect on the STO band gap or introduces detrimental midgap states except for Pd and Pt that are able to reduce the STO band gap. In contrast, doping S and Se significantly reduces STO’s direct band gap, thus, leading to appreciable optical absorption transitions in the visible spectral range. In this work, our findings provide that Pd-, S-, and Se-doped STO are potential promising photocatalysts for water splitting under visible light irradiation thereby providing insightful theoretical guides for experiments to improve the photocatalytic activity of STO.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Comparing event generator predictions and ab initio calculations of ν- 12 C neutral-current quasielastic scattering at 1 GeV

The measurement of neutrino oscillations and exotic physics searches are important parts of the physics program in the near future, with new state-of-the-art experiments planned within the next decade. Future and modern experiments in these fields will make use of nuclear targets. Event generators (EGs) are software used in the analysis of neutrino oscillation experiments. EGs are used to predict kinematic observables for a range of neutrino energies. These simulations make use of simple models of nucleon dynamics. As such, they may fail to capture features of more rigorous theoretical calculations. This work compares EG performance to nuclear theory calculations by comparing observables generated in the two frameworks. We provide a common set of definitions between theory and experiment and assess the adequacy of the implementation of two nuclear physics models in EG simulations. Neutral-current quasielastic (NCQE) scattering events for neutrinos and antineutrinos on a 12 C target are simulated with a specific EG, NEUT, used by the T2K experiment for its analysis. The simulated cross sections are compared to analytic calculations from nuclear theory within the factorization scheme. We compare the NEUT implementation of two different models on nuclear spectral functions: the relativistic Fermi gas (RFG) and the correlated basis spectral function (CBF) to analytic calculations of the same models in the factorization scheme. For both nuclear physics models, we compare the appearance of features in the distributions relevant to experimental analyses. The peak of the cross section dσ/(dΩ dω) is consistent in energy transfer, ω, for RFG and CBF simulations. Qualitatively, the shape of the simulated distribution is similar to the one obtained through theory calculations; however, there are some discrepancies between the theory calculations and the NEUT simulation. While the EG simulations and analytic calculations with the same model of nuclear dynamics show similar overall features, there are still differences between the two. These results demonstrate the importance of benchmarking EGs so their nuclear physics implementations can be improved for the analysis of future experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Revealing Nanoscale Chemical Heterogeneities in Polycrystalline Mo-BiVO 4 Thin Films

The activity of polycrystalline thin film photoelectrodes is impacted by local variations of the material properties due to the exposure of different crystal facets and the presence of grain/domain boundaries. Here a multi-modal approach is applied to correlate nanoscale heterogeneities in chemical composition and electronic structure with nanoscale morphology in polycrystalline Mo-BiVO 4 . By using scanning transmission X-ray microscopy, the characteristic structure of polycrystalline film is used to disentangle the different X-ray absorption spectra corresponding to grain centers and grain boundaries. Comparing both spectra reveals phase segregation of V 2 O 5 at grain boundaries of Mo-BiVO 4 thin films, which is further supported by X-ray photoelectron spectroscopy and many-body density functional theory calculations. Theoretical calculations also enable to predict the X-ray absorption spectral fingerprint of polarons in Mo-BiVO 4 . After photo-electrochemical operation, the degraded Mo-BiVO 4 films show similar grain center and grain boundary spectra indicating V 2 O 5 dissolution in the course of the reaction. Overall, these findings provide valuable insights into the degradation mechanism and the impact of material heterogeneities on the material performance and stability of polycrystalline photoelectrodes.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Spectroscopic and computational investigations of organometallic complexation of group 12 transition metals by methanobactins from Methylocystis sp. SB2

Methanotrophic bacteria catalyze the aerobic oxidation of methane to methanol using Cu-containing enzymes, thereby exerting a modulating influence on the global methane cycle. To facilitate the acquisition of Cu ions, some methanotrophic bacteria secrete small modified peptides known as “methanobactins,” which strongly bind Cu and function as an extracellular Cu recruitment relay, analogous to siderophores and Fe. In addition to Cu, methanobactins form complexes with other late transition metals, including the Group 12 transition metals Zn, Cd, and Hg, although the interplay among solution-phase configurations, metal interactions, and the spectroscopic signatures of methanobactin-metal complexes remains ambiguous. In this study, the complexation of Zn, Cd, and Hg by methanobactin from Methylocystis sp. strain SB2 was studied using a combination of absorbance, fluorescence, extended x-ray absorption fine structure (EXAFS) spectroscopy, and time-dependent density functional theory (TD-DFT) calculations. We report changes in sample absorbance and fluorescence spectral dynamics, which occur on a wide range of experimental timescales and characterize a clear stoichiometric complexation dependence. Mercury L3-edge EXAFS and TD-DFT calculations suggest a linear model for Hg--S coordination, and TD-DFT suggests a tetrahedral model for Zn 2+ and Cd 2+ . We observed an enhancement in the fluorescence of methanobactin upon interaction with transition metals and propose a mechanism of complexation-hindered isomerization drawing inspiration from the wild-type Green Fluorescent Protein active site. Collectively, our results represent the first combined computational and experimental spectroscopy study of methanobactins and shed new light on molecular interactions and dynamics that characterize complexes of methanobactins with Group 12 transition metals.

59 BASIC BIOLOGICAL SCIENCES↗