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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

All-Order Full-Coulomb Quantum Spectral Line-Shape Calculations

Understanding how atoms interact with hot dense matter is essential for astrophysical and laboratory plasmas. Interactions in high-density plasmas broaden spectral lines, providing a rare window into interactions that govern, for example, radiation transport in stars. However, up to now, spectral line-shape theories employed at least one of three common approximations: second-order Taylor treatment of broadening operator, dipole-only interactions between atom and plasma, and classical treatment of perturbing electrons. In this Letter, we remove all three approximations simultaneously for the first time and test the importance for two applications: neutral hydrogen and highly ionized magnesium and oxygen. Finally, we found 15%–50% change in the spectral line widths, which are sufficient to impact applications including white-dwarf mass determination, stellar-opacity research, and laboratory plasma diagnostics.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Spectral Narrowing Accompanies Enhanced Spatial Resolution in Saturated Coherent Anti-Stokes Raman Scattering (CARS): Comparisons of Experiment and Theory

Here, we demonstrate theoretically and confirm experimentally the mechanism by which spectral narrowing accompanies enhanced spatial resolution in a saturated coherent anti-Stokes Raman scattering (CARS) signal that is demodulated at the third harmonic (3$f$) of the pump modulation frequency ($f$). Under these modulation conditions, theory predicts a narrowing of the full-width at half-maximum (FWHM) of the CARS spectrum by a factor of 2.0 with respect to that of the spectrum obtained by demodulation at the fundamental frequency. Theory also predicts an improvement of spatial resolution by a factor of 1.7. Experimentally, narrowing of the FWHM of the CARS spectrum of 1,4-bis((E)-2-methylstyryl) benzene (MSB) crystals by a factor of 2.5 is observed upon saturation. Further experimental confirmation is provided from investigating diamond particles, for which spectral narrowing was enhanced by a factor of 2.8 and spatial resolution was enhanced by a factor of 2. Details of the mechanism and execution of the saturated CARS experiment are elucidated and limits to its applicability are suggested, one of which is the conclusion that the saturation approach is not suitable for extraction of harmonics beyond 3$f$ . In this work we have developed a more comprehensive understanding of the correlation between the observed experimental results and experimental factors than has been previously reported.

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

Second-order spectral line shift comparisons

The second-order spectral line width formulae from the projection operator and kinetic theory methods were recently compared. It was shown that a systematic expansion of the projection operator width expression including initial correlations formally agrees with the second-order kinetic theory result. It is now shown that the second-order dynamic shifts are also formally the same. The static shifts, however, differ due to an ad hoc treatment of electron-electron correlations in the projection operator method. The approximation is necessary in order to screen the radiator-electron interactions. The differences, however, are expected to be small. Finally, the results suggest using the rigorous and more compact second-order width and shift expressions from the kinetic theory method as the starting point for spectral line shape calculations. At line center, however, the projection operator second-order expression for the width and shift simplifies and reduces to the kinetic theory result.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Spectral properties and enhanced superconductivity in renormalized Migdal-Eliashberg theory

Migdal-Eliashberg theory describes the properties of the normal and superconducting states of electron-phonon-mediated superconductors based on a perturbative treatment of the electron-phonon interactions. It is necessary to include both electron and phonon self-energies self-consistently in Migdal-Eliashberg theory in order to match numerically exact results from determinantal quantum Monte Carlo in the adiabatic limit. Here in this work we provide a method to obtain the real-axis solutions of the Migdal-Eliashberg equations with electron and phonon self-energies calculated self-consistently. Our method avoids the typical challenge of computing cumbersome singular integrals on the real axis and is numerically stable and exhibits fast convergence. Analyzing the resulting real-frequency spectra and self-energies of the two-dimensional Holstein model, we find that self-consistently including the lowest-order correction to the phonon self-energy significantly affects the solution of the Migdal-Eliashberg equations. The calculation captures the broadness of the spectral function, renormalization of the phonon dispersion, enhanced effective electron-phonon coupling strength, minimal increase in the electron effective mass, and the enhancement of superconductivity which manifests as a superconducting ground state despite strong competition with charge-density-wave order. We discuss surprising differences in two common definitions of the electron-phonon coupling strength derived from the electron mass and the density of states, quantities which are accessible through experiments such as angle-resolved photoemission spectroscopy and electron tunneling. An approximate upper bound on 2Δ/T c for conventional superconductors mediated by retarded electron-phonon interactions is proposed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Resonant inelastic x-ray scattering in the topological semimetal FeSi

The energy spectrum of topological semimetals contains protected degeneracies in reciprocal space that correspond to Weyl, Dirac, or multifold fermionic states. To exploit the unconventional properties of these states, one has to access the electronic structure of the three-dimensional bulk. In this paper, we present a joint theory-experiment study of the electronic structure of a candidate topological semimetal with resonant inelastic x-ray scattering (RIXS). We resolve the bulk electronic states of FeSi using momentum-dependent RIXS at the Fe L 3 edge. We observe a broad excitation continuum devoid of sharp features, consistent with particle-hole scattering in an underlying electronic band structure. Using density functional theory (DFT), we calculate the electronic structure of FeSi and derive a band theory formulation of RIXS in the fast collision approximation to model the scattering process with zero adjustable parameters. While band theory predicts an excitation continuum with broad spectral features similar to the observed ones, discrepancies between theory and experiment suggest the presence of low-energy processes that DFT alone does not account for. Further, this study of RIXS in a topological semimetal shows that RIXS is a useful tool for revealing unanticipated behavior of bulk electronic states in this class of materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Spectral Threshold for Extremal Cyclic Edge-Connectivity

In this report, the cyclic edge-connectivity of a graph G is the least k such that there exists a set of k edges whose removal disconnects G into components where every component contains a cycle. We show that for graphs of minimum degree at least 3 and girth g at least 4, the cyclic edge-connectivity is bounded above by (Δ-2)g where Δ is the maximum degree. We then prove that if the second eigenvalue of the adjacency matrix of a d-regular graph of girth g ≥ 4 is sufficiently small, then the cyclic edge-connectivity is (d-2)g, providing a spectral condition for when this upper bound on cyclic edge-connectivity is tight.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2022

Spectroscopic investigation of the electronic and excited state properties of para-substituted tetraphenyl porphyrins and their electrochemically generated ions

Porphyrins play pivotal roles in many crucial biological processes including photosynthesis. However, there is still a knowledge gap in understanding electronic and excited state implications associated with functionalization of the porphyrin ring system. These effects can have electrochemical and spectroscopic signatures that reveal the complex nature of these somewhat minor substitutions, beyond simple inductive or electronic effect correlations. To obtain a deeper insight into the influences of porphyrin functionalization, four free-base, meso-substituted porphyrins: tetraphenyl porphyrin (TPP), tetra(4-hydroxyphenyl) porphyrin (THPP), tetra(4-carboxyphenyl) porphyrin (TCPP), and tetra(4-nitrophenyl) porphyrin (TNPP), were synthesized, characterized, and investigated. The influence of various substituents, (-hydroxy,-carboxy, and -nitro) in the para position of the meso-substituted phenyl moieties were evaluated by spectroelectrochemical techniques (absorption and fluorescence), femtosecond transient absorption spectroscopy, cyclic and differential pulse voltammetry, ultraviolet photoelectron spectroscopy (UPS), and time-dependent density functional theory (TD-DFT). Spectral features were evaluated for the neutral porphyrins and differences observed among the various porphyrins were further explained using rendered frontier molecular orbitals pertaining to the relevant transitions. Electrochemically generated anionic and cationic porphyrin species indicate similar absorbance spectroscopic signatures attributed to a red-shift in the Soret band. Emissive behavior reveals the emergence of one new fluorescence decay pathway for the ionic porphyrin, distinct from the neutral macrocycle. Femtosecond transient absorption spectroscopy analysis provided further analysis of the implications on the excited-state as a function of the para substituent of the free-base meso-substituted tetraphenyl porphyrins. Herein, we provide an in-depth and comprehensive analysis of the electronic and excited state effects associated with systematically varying the induced dipole at the methine bridge of the free-base porphyrin macrocycle and the spectroscopic signatures related to the neutral, anionic, and cationic species of these porphyrins.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Modeling Si/SiGe quantum dot variability induced by interface disorder reconstructed from multiperspective microscopy

SiGe heteroepitaxial growth yields pristine host material for quantum dot qubits, but residual interface disorder can lead to qubit-to-qubit variability that might pose an obstacle to reliable SiGe-based quantum computing. By convolving data from scanning tunneling microscopy and high-angle annular dark field scanning transmission electron microscopy, we reconstruct 3D interfacial atomic structure and employ an atomistic multi-valley effective mass theory to quantify qubit spectral variability. The results indicate (1) appreciable valley splitting (VS) variability of ~50% owing to alloy disorder and (2) roughness-induced double-dot detuning bias energy variability of order 1–10 meV depending on well thickness. For measured intermixing, atomic steps have negligible influence on VS, and uncorrelated roughness causes spatially fluctuating energy biases in double-dot detunings potentially incorrectly attributed to charge disorder. Our approach yields atomic structure spanning orders of magnitude larger areas than post-growth microscopy or tomography alone, enabling more holistic predictions of disorder-induced qubit variability.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Graph Metric Learning Quantifies Morphological Differences between Two Genotypes of Shoot Apical Meristem Cells in Arabidopsis

We present a method for learning “spectrally descriptive” edge weights for graphs. We generalize a previously known distance measure on graphs (Graph Diffusion Distance), thereby allowing it to be tuned to minimize an arbitrary loss function. Because all steps involved in calculating this modified GDD are differentiable, we demonstrate that it is possible for a small neural network model to learn edge weights which minimize loss. We apply this method to discriminate between graphs constructed from shoot apical meristem images of two genotypes of Arabidopsis thaliana specimens: wild-type and trm678 triple mutants with cell division phenotype. Training edge weights and kernel parameters with contrastive loss produces a learned distance metric with large margins between these graph categories. We demonstrate this by showing improved performance of a simple k-nearest-neighbors classifier on the learned distance matrix. We also demonstrate a further application of this method to biological image analysis. Once trained, we use our model to compute the distance between the biological graphs and a set of graphs output by a cell division simulator. Comparing simulated cell division graphs to biological ones allows us to identify simulation parameter regimes which characterize mutant vs. wild-type Arabidopsis cells. We find that trm678 mutant cells are characterized by increased randomness of division planes and decreased ability to avoid previous vertices between cell walls.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Coherency-Constrained Spectral Clustering for Power Network Reduction

This paper presents a methodology for reducing the complexity of large-scale power network models using spectral clustering, aggregation of electrical components, and cost function approximation. Two approaches are explored using unconstrained and constrained spectral clustering to determine areas for effective system reduction. Once the system areas are determined, both loads and generators by type are aggregated, and their new cost function is approximated through polynomial curve-fitting or statistical methods. The performance of reduced networks is evaluated in terms of their ability to follow the true daily cost of the original system over a 24-hour period considering a set of several days. Two test systems are taken as test beds. Application of the methodology to a modified version of the IEEE 39-bus system reduces it from 17 generators to a 4-bus system and 9 generators with about 93% of accuracy. Similarly, the IEEE 118-bus system is reduced from 19 generators to a 3-bus system with three aggregated units achieving over 99% of accuracy. These findings address scalability challenges and enhance accuracy for high and mid-loading level conditions, and by aggregating thermal units with similar cost functions.

42 ENGINEERING↗
DOE OSTI2022

On the structure of isometrically embeddable metric spaces

Since its popularization in the 1970s, the Fiedler vector of a graph has become a standard tool for clustering of the vertices of the graph. Recently, Mendel and Noar, Dumitriu and Radcliffe, and Radcliffe and Williamson have introduced geometric generalizations of the Fiedler vector. Motivated by questions stemming from their work, we provide structural characterizations for when a finite metric space can be isometrically embedded in a Hilbert space.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2024

Unifying Combinatorial and Graphical Methods in Artificial Intelligence

Recently, a new graph Laplacian, called the inner product Laplacian, was introduced which generalizes many existing Laplacians, including the normalized and combinatorial Laplacian and their weighted variants. The key observation behind the inner product Laplacian is that by defining appropriate inner product spaces on the vertices and edges, the standard Laplacians can be recovered as Hodge Laplacians over the simplicial complex formed by the edges and vertices. These inner product spaces form a natural way to incorporate non-combinatorial information into the definition of a domain-specific Laplacian. In particular, in contrast to current domain-specific weighting schemes which rely solely on edge weights, information regarding the similarity of non-adjacent vertices and arbitrary pairs of edges can be effectively incorporated into the Laplacian. In order to illustrate this approach we consider the problem of calculating the potential energy of an atomistic configuration using Graph Neural Networks. In comparison with start-of-the-art approaches, such as SchNet, our approach replaces a learned (via auto-encoder) representation of the atom types with an inner product space on atoms based on scientific knowledge (e.g., electronegativity). We will illustrate how this approach captures key chemical properties of the molecules and compare the energy calculations with state-of-the-art neural network approaches. However, to compute the resulting Laplacian involves a mixture of sparse and dense matrix computation and yields a dense matrix as the basis for the graph convolution. This dense convolutional kernel necessitates moving away from the standard message passing framework for graph neural networks and increases the computational cost of applying the kernel. In order to mitigate these costs we investigate means of leveraging the mixed sparse and dense computations to reduce the overall computational cost and how these approaches can be automatically transferred to energy efficient hardware (e.g., field programmable gate arrays (FPGAs)).

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2022

Unexpected features in the optical vibrational spectra of δ-UO 3

Uranium trioxide displays a complex chemical phase space, with at least six structurally distinct polymorphs accessible via different synthetic routes. Remarkably, despite its technological importance, full structural and electronic characterization of these polymorphs remains an open area of study. δ-UO 3 in particular has attracted significant theoretical attention due to its high point group and space group symmetries, having U (VI) in octahedral coordination with polyhedra interconnected through corner-sharing to build a 3-D cubic lattice with space group symmetry Pm-3m and Z = 1. Critical experimental information, such as its optical vibrational spectra, are not known. Here, we study the Raman and infrared (IR) spectra of δ-UO 3 together with the support of density functional theory (DFT) calculations for spectral interpretation. A symmetry analysis of the DFT-predicted phonon eigenmodes indicates that δ-UO 3 should have two IR active modes and no Raman active modes. Experimental results, however, indicate significant Raman scattering from δ-UO 3 . We therefore propose four potential explanations for this apparent contradiction: a possible tetragonal distortion to the cubic cell, the existence of a surface impurity layer, vacancy scattering, and structural activation of Raman signal. We use powder X-ray diffraction and confocal Raman spectroscopy with depth profiling to investigate these possibilities and suggest future experiments to explore this phenomenon in more detail. Understanding the lattice dynamics of δ-UO 3 is important for identification of technogenic U phases via Raman and infrared spectroscopy and our results indicate that the simple understanding of δ-UO 3 as a high-symmetry cubic structure should be reconsidered.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2021

Electronic structure of Alq 3 and Liq using soft X-ray spectroscopy and density functional theory calculation

We show the electronic structure of aluminum tris-8-hydroxyquinoline (Alq 3 ) and 8-hydroquinolatolithium (Liq) was investigated using a combination of X-ray emission spectroscopy (XES), X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS), and spectral simulation with density functional theory. The chemical bonding states of Alq 3 and Liq were analyzed using XPS core-level spectra. The band gaps of Alq 3 and Liq were measured by combining the XAS and XES results. Additionally, resonant and non-resonant XES were used to measure the density of states for O sites in the molecules.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Simulation of Stark-broadened Hydrogen Balmer-line Shapes for DA White Dwarf Synthetic Spectra

Abstract White dwarfs (WDs) are useful across a wide range of astrophysical contexts. The appropriate interpretation of their spectra relies on the accuracy of WD atmosphere models. One essential ingredient of atmosphere models is the theory used for the broadening of spectral lines. To date, the models have relied on Vidal et al., known as the unified theory of line broadening (VCS). There have since been advancements in the theory; however, the calculations used in model atmosphere codes have only received minor updates. Meanwhile, advances in instrumentation and data have uncovered indications of inaccuracies: spectroscopic temperatures are roughly 10% higher and spectroscopic masses are roughly 0.1 M ⊙ higher than their photometric counterparts. The evidence suggests that VCS-based treatments of line profiles may be at least partly responsible. Gomez et al. developed a simulation-based line-profile code Xenomorph using an improved theoretical treatment that can be used to inform questions around the discrepancy. However, the code required revisions to sufficiently decrease noise for use in model spectra and to make it computationally tractable and physically realistic. In particular, we investigate three additional physical effects that are not captured in the VCS calculations: ion dynamics, higher-order multipole expansion, and an expanded basis set. We also implement a simulation-based approach to occupation probability. The present study limits the scope to the first three hydrogen Balmer transitions (H α , H β , and H γ ). We find that screening effects and occupation probability have the largest effects on the line shapes and will likely have important consequences in stellar synthetic spectra.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

The shear Alfvén continuum of quasisymmetric stellarators

The shear Alfvén wave (SAW) continuum plays a critical role in the stability of energetic particle-driven Alfvén eigenmodes. We develop a theoretical framework to analyze the SAW continuum in three-dimensional (3-D) quasisymmetric magnetic fields, focusing on its implications for stellarator design. By employing a near-axis model and degenerate perturbation theory, the continuum equation is solved, highlighting unique features in 3-D configurations, such as the interactions between spectral gaps. Numerical examples validate the theory, demonstrating the impact of flux-surface shaping and quasisymmetric field properties on continuum structure. The results provide insights into optimizing stellarator configurations to minimize resonance-driven losses of energetic particles. This work establishes a basis for incorporating Alfvénic stability considerations into the stellarator design process, demonstrated through optimization of a quasihelical configuration to avoid high-frequency spectral gaps.

fusion plasma↗
DOE OSTI2021

Phenomenology of Spectral Functions in Disordered Spin Chains at Infinite Temperature

Studies of disordered spin chains have recently experienced a renewed interest, inspired by the question to which extent the exact numerical calculations comply with the existence of a many-body localization phase transition. For the paradigmatic random field Heisenberg spin chains, many intriguing features were observed when the disorder is considerable compared to the spin interaction strength. Here, we introduce a phenomenological theory that may explain some of those features. The theory is based on the proximity to the noninteracting limit, in which the system is an Anderson insulator. Taking the spin imbalance as an exemplary observable, we demonstrate that the proximity to the local integrals of motion of the Anderson insulator determines the dynamics of the observable at infinite temperature. In finite interacting systems our theory quantitatively describes its integrated spectral function for a wide range of disorders.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

A precision test of averaging in AdS/CFT

We reconsider the role of wormholes in the AdS/CFT correspondence. We focus on Euclidean wormholes that connect two asymptotically AdS or hyperbolic regions with $\mathbb{S}$ 1 × $\mathbb{S}$ d-1 boundary. There is no solution to Einstein’s equations of this sort, as the wormholes possess a modulus that runs to infinity. To find on-shell wormholes we must stabilize this modulus, which we can do by fixing the total energy on the two boundaries. Such a wormhole gives the saddle point approximation to a non-standard problem in quantum gravity, where we fix two asymptotic boundaries and constrain the common energy. Crucially the dual quantity does not factorize even when the bulk is dual to a single CFT, on account of the fixed energy constraint. From this quantity we extract a smeared version of the microcanonical spectral form factor. For a chaotic theory this quantity is self-averaging, i.e. well-approximated by averaging over energy windows, or over coupling constants. We go on to give a precision test involving the microcanonical spectral form factor where the two replicas have slightly different coupling constants. In chaotic theories this form factor is known to smoothly decay at a rate universally predicted in terms of one replica physics, provided that there is an average either over a window or over couplings. We compute the expected decay rate for holographic theories, and the form factor from a wormhole, and the two exactly agree for a wide range of two-derivative effective field theories in AdS. This gives a precision test of averaging in AdS/CFT. Our results interpret a number of confusing facts about wormholes and factorization in AdS and suggest that we should regard gravitational effective field theory as a mesoscopic description, analogous to semiclassical mesoscopic descriptions of quantum chaotic systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗