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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Regulation of Alfvén Eigenmodes by Microturbulence in Fusion Plasmas

Global gyrokinetic simulations of mesoscale reversed shear Alfven eigenmodes (RSAE) excited by energetic particles (EP) in fusion plasmas find that RSAE amplitude and EP transport are much higher than experimental levels at nonlinear saturation, but quickly diminish to very low levels after the saturation when background microturbulence is artificially suppressed. In contrast, in simulations coupling micro-meso scales, the RSAE amplitude and EP transport decrease drastically at the initial saturation but later increases to the experimental levels in the quasi-steady state with bursty dynamics due to regulation by thermal ion temperature gradient (ITG) microturbulence. The quasi-steady state EP transport is larger for a stronger microturbulence. Here, the RSAE amplitude in the quasi-steady state ITG-RSAE turbulence from gyrokinetic simulations, for the first time, agrees very well with experimental measurements.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Magnon damping in the zigzag phase of the Kitaev-Heisenberg- Γ model on a honeycomb lattice

We calculate dispersions and damping of the magnetic excitations in the model that is relevant to a description of the magnetic properties of iridium oxides α-Li 2 IrO 3 and Na 2 IrO 3 , and Ru-based materials such as α-RuCl 3 . Focusing on the parameter regime with the zigzag spin pattern in the ground state that is consistent with experiments, we are able to obtain explicit analytical expressions for magnon energies and eigenstates and go beyond the standard linear spin-wave theory approximation by calculating magnon damping and demonstrating its role in the dynamical structure factor. Here, we show that the magnon damping effects in both Born and self-consistent approximations are very significant, underscoring the importance of nonlinear magnon coupling in interpreting broad features in the neutron-scattering spectra.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Thermal Processing Conditions for the Synthesis of Near Theoretical Density Li 5 La 3 Ta 2 O 12 Ceramics for Ceramic Dual-Mode Detectors

A family of Li-containing garnet compounds, extensively investigated for Li-ion solid electrolyte applications, show great potential to be developed into transparent ceramic dual-mode scintillators. In particular, Li 5 La 3 Ta 2 O 12 (LLTaO) shows promise as an efficient dual-mode scintillator due to its high Li content, high density, non-hygroscopicity, and high effective-Z. Often the synthesis of LLTaO ceramics involves solid state processing techniques starting with oxide and carbonate powders, calcining, sintering for the removal of residual porosity, and post-processing. This study focuses on two objectives: (1) establishing thermal processing boundary conditions for a flexible alkoxide-based sol-gel method for synthesizing fine-grained powders; and (2), consolidating powders via hot-pressing to form high-density ceramics. In this study, near single-phase ceramics were achieved by hot-pressing sol-gel powders with varying amounts of excess Li. Rietveld refinements were used to analyze X-ray diffraction data and provide a quantitative evaluation of the phases present in the hot pressed ceramics. Some of the diffraction data showed large low angle peak asymmetry, suggesting the presence of two cubic Li 5 La 3 Ta 2 O 12 garnet phases with different lattice parameters. Depending on the synthesis and processing conditions, the refinement revealed ~ 90 wt% concentration of a phase with a ≈ 12.8 Å and ~ 10 wt% concentration of a phase with a ≈ 12.9 Å, indicating a remaining excess of Li in the hot pressed ceramics in the large lattice parameter phase. These synthesis experiments allowed for the determination of a baseline for Li loss during hot-pressing. X-ray excited radioluminescence and photoluminescence excitation and emission spectra were obtained from the hot pressed ceramics. In conclusion, the measured emission spectra featured broad tantalate emission and line emissions likely from a rare-earth impurity.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Performance of high-order Godunov-type methods in simulations of astrophysical low Mach number flows

High-order Godunov methods for gas dynamics have become a standard tool for simulating different classes of astrophysical flows. Their accuracy is mostly determined by the spatial interpolant used to reconstruct the pair of Riemann states at cell interfaces and by the Riemann solver that computes the interface fluxes. In most Godunov-type methods, these two steps can be treated independently, so that many different schemes can in principle be built from the same numerical framework. Because astrophysical simulations often test out the limits of what is feasible with the computational resources available, it is essential to find the scheme that produces the numerical solution with the desired accuracy at the lowest computational cost. However, establishing the best combination of numerical options in a Godunov-type method to be used for simulating a complex hydrodynamic problem is a nontrivial task. In fact, formally more accurate schemes do not always outperform simpler and more diffusive methods, especially if sharp gradients are present in the flow. For this work, we used our fully compressible Seven-League Hydro (SLH) code to test the accuracy of six reconstruction methods and three approximate Riemann solvers on two- and three-dimensional (2D and 3D) problems involving subsonic flows only. We considered Mach numbers in the range from 10 −3 to 10 −1 , which are characteristic of many stellar and geophysical flows. In particular, we considered a well-posed, 2D, Kelvin–Helmholtz instability problem and a 3D turbulent convection zone that excites internal gravity waves in an overlying stable layer. Although the different combinations of numerical methods converge to the same solution with increasing grid resolution for most of the quantities analyzed here, we find that (i) there is a spread of almost four orders of magnitude in computational cost per fixed accuracy between the methods tested in this study, with the most performant method being a combination of a low-dissipation Riemann solver and a sextic reconstruction scheme; (ii) the low-dissipation solver always outperforms conventional Riemann solvers on a fixed grid when the reconstruction scheme is kept the same; (iii) in simulations of turbulent flows, increasing the order of spatial reconstruction reduces the characteristic dissipation length scale achieved on a given grid even if the overall scheme is only second order accurate; (iv) reconstruction methods based on slope-limiting techniques tend to generate artificial, high-frequency acoustic waves during the evolution of the flow; and (v) unlimited reconstruction methods introduce oscillations in the thermal stratification near the convective boundary, where the entropy gradient is steep.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Perspective on Many-Body Methods for Molecular Polaritonic Systems

Recent advances in strong light–matter interactions have revealed a wealth of new physical phenomena in molecules embedded in optical cavities, including modified chemical reactivity, altered excitation spectra, and novel quantum correlations. To describe these effects from first-principles, the field of ab initio quantum electrodynamics (QED) has emerged as a compelling extension of quantum chemistry that treats electronic and photonic degrees of freedom on equal footing. In this Perspective, we review the growing landscape of many-body QED methods, including Hartree–Fock, density functional theory (QEDFT), time-dependent DFT (QED-TDDFT), configuration interaction (QED-CI), complete active space (QED-CASSCF), coupled cluster (QED-CC), quantum Monte Carlo (QED-QMC), and density matrix renormalization group (QED-DMRG), highlighting recent developments and implementations. We further explore real-time methods, gradient and Hessian formalisms, and the integration of nonadiabatic nuclear dynamics. Applications range from benchmark simulations of polaritonic chemistry to quantum simulations on emerging quantum hardware. We conclude by outlining future directions for theory development and interdisciplinary efforts at the interface of quantum chemistry, condensed matter, and quantum optics.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Spin dynamics in quantum dots on liquid helium

Liquid He-4 is free from magnetic defects, making it an ideal substrate for electrons with long-lived spin states. Such states can serve as qubit states. Here, in this study, we consider the spin states of electrons electrostatically localized in quantum dots on a helium surface. Efficient gate operations in this system require spin-orbit coupling. It can be created by a nonuniform magnetic field from a current-carrying wire, can be turned on and off, and allows one to obtain large electrodipole moment and comparatively fast coupling of spins in neighboring dots. Of central importance is to understand spin decay due to the spin-orbit coupling. We establish the leading mechanism of such decay and show that the decay is sufficiently slow to enable high-fidelity single- and two-qubit gate operations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Revisiting excitation gaps in the fractional quantum Hall effect

Recent systematic measurements of the quantum well width dependence of the excitation gaps of fractional quantum Hall states in high mobility samples open the possibility of a better quantitative understanding of this important issue. Here we present what we believe to be accurate theoretical gaps including the effects of finite width and Landau level (LL) mixing. While theory captures the width dependence, there still remains a deviation between the calculated and the measured gaps, presumably caused by disorder. It is customary to model the experimental gaps of the n/(2n ± 1) states as Δ n/(2n+1) = Ce 2 /[(2n ± 1)ϵl]-Γ, where ϵ is the dielectric constant of the background semiconductor and l is the magnetic length; the first term is interpreted as the cyclotron energy of composite fermions and Γ as a disorder-induced broadening of composite-fermion LLs. Fitting the gaps for various fractional quantum Hall states, we find that Γ can be nonzero even in the absence of disorder.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Broken Luttinger theorem in the two-dimensional Fermi-Hubbard model

One of the fundamental questions about high-temperature cuprate superconductors is the size of the Fermi surface underlying the superconducting state. By analyzing the single-particle spectral function for the Fermi-Hubbard model as a function of repulsion U and chemical potential μ, we find that the Fermi surface in the normal state undergoes a transition from a large Fermi surface matching the Luttinger volume as expected in a Fermi liquid, to a Fermi surface that encloses fewer electrons that we dub the “Luttinger breaking” phase, as the Mott insulator is approached. This transition into a non-Fermi-liquid phase that violates the Luttinger count occurs at a critical density in the absence of any other broken symmetry. We obtain the Fermi-surface contour from the spectral weight A k (ω = 0) and from an analysis of the singularities of the Green's function Re G k (E = 0), calculated using determinantal quantum Monte Carlo and analytic continuation methods. We discuss our numerical results in connection with experiments on Hall measurements, scanning tunneling spectroscopy, and angle-resolved photoemission spectroscopy.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Modal Field Reconstruction in Resonant Cavities in the Fundamental and Undermoded Frequency Regimes

Theory, simulations, and experiments are presented that demonstrate reconstruction of electromagnetic fields in a cavity from sparse probe measurements. Such techniques are often referred to as virtual sensing, allowing fields at unobserved locations to be predicted. These methods are appropriate for the fundamental and undermoded regimes, providing the ability to estimate fields (and shielding effectiveness) throughout an arbitrarily shaped cavity from a few judiciously spaced probes. A modal simulation method is implemented that allows the response of arbitrarily shaped cavities to be rapidly computed with respect to varying probe locations and slot parameters, enabling statistical analysis of probe placement on reconstruction performance. A cylindrical vessel with numerous probe holes is developed for experiments, referred to as Perforated Vessel 2 (PV2). Experiments are performed on the vessel with and without a steel box inside, where transmit power is delivered into the vessel either through probes (probe injection) or through slots using an external antenna (slot excitation). Simulations and experiments illustrate that when the number of probes is minimal (equal to the number of mode coefficients to be estimated at each frequency), probe placement is critical to avoid missed peaks and to have acceptable reconstruction error. Probe placement becomes less important as the number of probes is increased, but care is still required to avoid probe locations giving poor performance.

42 ENGINEERING↗
DOE OSTI2022

State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Nonlinear spectroscopies can disentangle spectra that are congested due to inhomogeneous broadening. Here, in conjunction with theoretical calculations, attosecond extreme ultraviolet (XUV) four-wave-mixing (FWM) spectroscopy is utilized to probe the dynamics of autoionizing inner valence excited Rydberg states of the polyatomic molecule, CO 2 . This tabletop nonlinear technique employs a short attosecond XUV pulse train and two noncollinear, few-cycle near-infrared pulses to generate background-free XUV wave-mixing signals. FWM emission is observed from the n=5-7 states of the Henning sharp ndσ g Rydberg series that converges to the ionic $\widetilde{B}$ 2 Σ$^{+}_{u}$ state. However, these transient emission signals decay with lifetimes of 33 ± 6, 53 ± 2, and 94 ± 2 fs, respectively, which calculations show are consistent with the lifetimes of the short-lived n=6-8 members of the nsσ g character Henning diffuse Rydberg series. The oscillator strengths of transitions between states involved in all possible resonant FWM processes are calculated, verifying that the nonlinear spectra are dominated by pathways described by an initial excitation to the diffuse nsσ g Rydberg series and emission from the sharp ndσ g Rydberg series. The results substantiate not only that attosecond XUV FWM spectroscopy produces rigorous and meaningful measurements of ultrafast dynamics in polyatomic systems, but also that nonlinear spectroscopic techniques are versatile tools to selectively probe dynamics that are otherwise difficult to access.

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

Local Pair Natural Orbital-Based Coupled-Cluster Theory through Full Quadruples (DLPNO–CCSDTQ)

In this work, we implement a local pair natural orbitalbased coupled-cluster method through the full treatment of quadruple excitations (CCSDTQ). The domain-based local pair natural orbital (DLPNO) approach, which has successfully been applied to lower levels of coupled-cluster theory, is utilized in our algorithm, and thus our algorithm is called DLPNO-CCSDTQ. For simplicity in the working equations and in the implementation, we t 1 -dress the twoelectron integrals as well as Fock matrix elements. Our method can recover CCSDTQ-CCSDT and CCSDTQ-CCSDT(Q) energy differences on the order of 0.01−0.05 kcal mol −1 , even at a loose quadruples natural orbital (QNO) occupation number cutoff of 3.33 × 10 −6 . To highlight the capabilities of our code and its potential future applications, we showcase computations that would be intractable with canonical CCSDTQ, such as the benzene dimer, (H 2 O) 17 , and adamantane. With sufficient computing resources, computations up to 15 heavy atoms (40 atoms overall) may be feasible for fully bonded 3D systems.

Cluster chemistry↗
DOE OSTI2022

High-resolution CH stretch spectroscopy of jet-cooled cyclopentyl radical: First insights into equilibrium structure, out-of-plane puckering, and IVR dynamics

First, high-resolution sub-Doppler infrared spectroscopic results for cyclopentyl radical (C 5 H 9 ) are reported on the α-CH stretch fundamental with suppression of spectral congestion achieved by adiabatic cooling to T rot ≈ 19(4) K in a slit jet expansion. Surprisingly, cyclopentyl radical exhibits a rotationally assignable infrared spectrum, despite 3N – 6 = 36 vibrational modes and an upper vibrational state density (ρ ≈ 40–90 #/cm –1 ) in the critical regime (ρ ≈ 100 #/cm –1 ) necessary for onset of intramolecular vibrational relaxation (IVR) dynamics. Such high-resolution data for cyclopentyl radical permit detailed fits to a rigid-rotor asymmetric top Hamiltonian, initial structural information for ground and vibrationally excited states, and opportunities for detailed comparison with theoretical predictions. Specifically, high level ab initio calculations at the coupled-cluster singles, doubles, and perturbative triples (CCSD(T))/ANO0, 1 level are used to calculate an out-of-plane bending potential, which reveals a C 2 symmetry double minimum 1D energy surface over a C 2v transition state. Here, the inversion barrier [V barrier ≈ 3.7(1) kcal/mol] is much larger than the effective moment of inertia for out-of-plane bending, resulting in localization of the cyclopentyl wavefunction near its C 2 symmetry equilibrium geometry and tunneling splittings for the ground state too small (<1 MHz) to be resolved under sub-Doppler slit jet conditions. The persistence of fully resolved high-resolution infrared spectroscopy for such large cyclic polyatomic radicals at high vibrational state densities suggests a “deceleration” of IVR for a cycloalkane ring topology, much as low frequency torsion/methyl rotation degrees of freedom have demonstrated a corresponding “acceleration” of IVR processes in linear hydrocarbons.

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

Low-temperature breakdown of many-body perturbation theory for thermodynamics

It is shown analytically and numerically that the finite-temperature many-body perturbation theory in the grand canonical ensemble has zero radius of convergence at zero temperature when the energy ordering or degree of degeneracy for the ground state changes with the perturbation strength. When the degeneracy of the reference state is partially or fully lifted at the first-order Hirschfelder-Certain degenerate perturbation theory, the grand potential and internal energy diverge as T → 0. Contrary to earlier suggestions of renormalizability by the chemical potential μ, this nonconvergence, first suspected by W. Kohn and J. M. Luttinger, is caused by the nonanalytic nature of the Boltzmann factor e –E/k e T at T = 0, also plaguing the canonical ensemble, which does not involve chemical potential. The finding reveals a fundamental flaw in perturbation theory, which is deeply rooted in the mathematical limitation of power-series expansions and is unlikely to be removed within its framework.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Multifrequency eddy-current detection of fast transient thermal signatures for in situ monitoring applications

Eddy-current (EC) nondestructive evaluation has a long history of use in a variety of ex situ defect monitoring applications because of its exquisite sensitivity to local material variations. Due to the relationship between a material's conductivity and its temperature, EC methods have also been used to investigate quasistatic, long-range temperature variations in casting applications. However, these techniques remain underutilized for the measurement of rapidly varying, spatially nonuniform temperature distributions. In this work, we construct a model system capable of generating repeatable temperature transients in steel plates and measure real-time eddy-current signals with millisecond time resolution and spatial resolution of the order of 1 mm. Using a combination of Multiphysics simulations, fast thermal imaging, and time-resolved holographic interferometry, we tease apart contributions to the eddy-current signals arising from temperature variations and transient plate deformation. Finally, we perform a systematic study in which we vary the plate thickness and the eddy-current excitation frequency to demonstrate that eddy-current techniques can provide information about a three-dimensional, time-varying, subsurface thermal distribution, which is inaccessible to the traditional thermal imaging techniques.

Rosenberg, Ethan R. [Lawrence Livermore National L↗
DOE OSTI2025

Diverse Manifestations of Electron-Phonon Coupling in a Kagome Superconductor

Recent angle-resolved photoemission spectroscopy (ARPES) experiments on the kagome metal CsV_{3}Sb_{5} revealed distinct multimodal dispersion kinks and nodeless superconducting gaps across multiple electron bands. The prominent photoemission kinks suggest a definitive coupling between electrons and certain collective modes, yet the precise nature of this interaction and its connection to superconductivity remain to be established. Here, employing the state-of-the-art ab initio many-body perturbation theory computation, we present direct evidence that electron-phonon (e-ph) coupling induces the multimodal photoemission kinks in CsV_{3}Sb_{5}, and profoundly, drives the nodeless s-wave superconductivity, showcasing the diverse manifestations of the e-ph coupling. Our calculations well capture the experimentally measured kinks and their fine structures, and reveal that vibrations from different atomic species dictate the multimodal behavior. Results from anisotropic GW-Eliashberg equations predict a phonon-mediated superconductivity with nodeless s-wave gaps, in excellent agreement with various ARPES and scanning tunneling spectroscopy measurements. Despite the universal origin of the e-ph coupling, the contributions of several characteristic phonon vibrations vary in different phenomena, highlighting a versatile role of e-ph coupling in shaping the low-energy excitations of kagome metals.

Electron-phonon coupling↗
DOE OSTI2024

Dynamics of vacancy-induced modes in the non-Abelian Kitaev spin liquid

Here, we study the dynamical response of vacancy-induced quasiparticle excitations in the site-diluted Kitaev spin liquid with a magnetic field. Due to the flux-binding effect and the emergence of dangling Majorana fermions around each spin vacancy, the low-energy physics is governed by a set of vacancy-induced quasi-zero-energy modes. These localized modes result in unique characteristics of the dynamical spin correlation functions, which intriguingly mimic the single-quasiparticle density of states and further exhibit a quasi-zero-frequency peak. By recognizing the potential observability of these local correlation functions via scanning tunneling microscopy (STM), we show how the STM response is sensitive to the local flux configuration, the magnetic field strength, and the vacancy concentration. Constructing a simple model of the localized modes, we also elucidate how the local correlation functions can be interpreted in terms of the hybridization between these modes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Regional Source-Type Discrimination Using Nonlinear Alignment Algorithms

The discrimination problem in seismology aims to accurately classify different underground source types based on local, regional, and/or teleseismic observations of ground motion. Typical discriminant approaches are rooted in fundamental, physics-based differences in radiation pattern or wave excitation, which can be frequency-dependent and may not make use of the full waveform. In this article, we explore whether phase and amplitude distances derived from dynamic time warping (DTW) and elastic shape analysis (ESA) can inform event discrimination. We demonstrate the ability to distinguish underground point sources using synthetic waveforms calculated for a 1D Earth model and various source mechanisms. We then apply the method to recorded data from events in the Korean Peninsula, which includes declared nuclear explosions, a collapse event, and naturally occurring earthquakes. Phase and amplitude distances derived from DTW and ESA are then used to classify the event types via dendrogram and k-nearest-neighbor clustering analyses. Using information from the full waveform, we show how different underground sources can be distinguished at regional distances. We highlight the potential of these nonlinear alignment algorithms for discrimination and comment on ways we can extend the framework presented here.

58 GEOSCIENCES↗
DOE OSTI2024

Electronic Structure of Excitons in Hematite Fe 2 O 3

We present a computational study of the electronic structure of excitons in hematite Fe 2 O 3 using density functional theory (DFT) and time-dependent DFT theory. Excitons resulting from solar light absorption are precursors to photogenerated charge carriers, which are the active species in solar-to-fuel redox conversions. Upon vertical excitation, the lowest energy exciton is found to have a multideterminantal wave function, describing an electron excited from O 2p states to Fe 3d states of the nearest basal plane, possibly supporting a recent XUV-derived exciton structure with a radius of a single Fe–O bond. Subsequently, the exciton self-traps into stable electron–hole pair structures whose wave functions are well-approximated by single excitations conveniently labeled “HOMO–LUMO”. Self-trapping yields electron–hole pair structures whereby the electron state (electron polaron-like) is separated from the hole state (hole polaron-like) by 3, 5, 7, 9, ... basal planes in structures referred to as Exc-3, Exc-5, Exc-7, Exc-9, ... The natural transition orbitals (electron–hole states) exhibit a strong “localized” character. The hole state is best described as a (FeO 6 ) + octahedral moiety carrying ~0.65 h + charge, and overall ~70% of the hole is assigned to O 2p atomic states, mostly on the four (4) equatorial O atoms of the moiety. The electron state is best described as a (FeFe) – moiety carrying ~0.80 e – charge in Fe 3d atomic states. The lattice distortions around the hole site exhibit Fe–O bond shortening due to the removal of electron density from an orbital state with O–Fe–O antibonding character. The electron site shows Fe–Fe distance shortening due to excess electron density added to an orbital state with in-phase Fe–Fe interactions. Furthermore, these excitonic structures with increasing electron–hole separation can be viewed as the onset of exciton separation into isolated electrons and hole polarons.

36 MATERIALS SCIENCE↗