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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 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Multipoint Observations of Dispersive Scale Alfvénic Field‐Line Resonances Associated With Substorm Auroral Beads

We present a case study of the field-aligned current (FAC) systems that transpire within the high-altitude auroral acceleration region of an “auroral bead” initiated double oval substorm observed on 23 February 2001 by the Cluster fleet. Conjunctive Cluster measurements and auroral images from IMAGE reveal that auroral bead current system formation and evolution is a multi-scale, injection-mediated process. The FACs at large scales vary on substorm evolution time scales (~minutes) in response to the injection and evolution of hotter denser magnetospheric plasma. Embedded within the large-scale FACs are intense short-scale (≲ few 10s of km) currents comprising dispersive scale Alfvén wave (DAW) fluctuations. The DAWs are a complex mixture of ingoing and reflected components that regularly interfere to form a broad spectrum of kinetic (dispersive) scale Alfvénic field-line resonances (KFLRs). The Alfvénic currents appear as a nested series of upward and downward FAC densities with amplitudes reaching a few 100 nA/m 2 . Energized field-aligned or counterstreaming electrons near keV energies and below are observed with parallel skews that vary in concert with variations in the DAW current sense. Positive correlations between DAW electric field energy densities and the energies of energized H + , He + , and O + outflow are observed, indicative of ion energization within the DAW fields. Due to their L-shell location (L~5.8–7.0) and associations with injections, the KFLRs are interpreted as the high-altitude auroral zone analog of KFLRs observed in the equatorial inner magnetosphere.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Rotational excitations in rare-earth nuclei: A comparative study within three cranking models with different mean fields and treatments of pairing correlations

High-spin rotational bands in rare-earth Er (Z = 68), Tm (Z = 69), and Yb (Z = 70) isotopes are investigated by three different nuclear models. These are (i) the cranked relativistic Hartree-Bogoliubov (CRHB) approach with approximate particle number projection by means of the Lipkin-Nogami (LN) method, (ii) the cranking covariant density functional theory (CDFT) with pairing correlations treated by a shell-model-like approach (SLAP) or the so-called particle-number conserving (PNC) method, and (iii) cranked shell model (CSM) based on the Nilsson potential with pairing correlations treated by the PNC method. A detailed comparison between these three models in the description of the ground-state rotational bands of even-even Er and Yb isotopes is performed. The similarities and differences between these models in the description of the moments of inertia, the features of band crossings, and equilibrium deformations and pairing energies of the even-even nuclei under study are discussed. These quantities are considered as a function of rotational frequency and proton and neutron numbers. The changes in the properties of the first band crossings with increasing neutron number in this mass region are investigated. On average, a comparable accuracy of the description of available experimental data is achieved in these models. However, the differences between model predictions become larger above the first band crossings. Because of the time-consuming nature of numerical calculations in the CDFT-based models, a systematic study of the rotational properties of both ground-state and excited-state bands in odd-mass Tm nuclei is carried out only by the PNC-SCM. With few exceptions, the rotational properties of experimental 1-quasiparticle and 3-quasiparticle bands in 165,167,169,171 Tm are reproduced reasonably well. As a result, the appearance of backbendings or upbendings in these nuclei is well understood from the analysis of the variations of the occupation probabilities of the single-particle states and their contributions to total angular momentum alignment with rotational frequency.

150 ≤ A ≤ 189↗
DOE OSTI2022

The symmetric quasi-classical model using on-the-fly time-dependent density functional theory within the Tamm–Dancoff approximation

The primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavourable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like time-dependent density functional theory within the Tamm–Dancoff approximation (TDDFT/TDA), alleviate this cost for moderately sized molecular systems simulated on realistic time scales. Although TDDFT/TDA does have some limitations in accuracy, an appealing feature is that, in addition to including electron correlation through the use of a density functional, the cost of calculating analytic nuclear gradients and nonadiabatic coupling vectors is often computationally feasible even for moderately sized basis sets. Here in this work, some of the benefits and limitations of TDDFT/TDA are discussed and analysed with regard to its applicability as a ‘back-end’ electronic structure method for the symmetric quasi-classical Meyer–Miller model (SQC/MM). In order to investigate the benefits and limitations of TDDFT/TDA, SQC/MM is employed to predict and analyse a prototypical example of excited-state hydrogen transfer in gas-phase malonaldehyde. Then, the ring-opening dynamics of selenophene are simulated, which highlight some of the deficiencies of TDDFT/TDA. Additionally, some new algorithms are proposed that speed up the calculation of analytic nuclear gradients and nonadiabatic coupling vectors for a set of excited electronic states.

molecular dynamics↗
DOE OSTI2022

Multi-GeV Electron Bunches from an All-Optical Laser Wakefield Accelerator

We present the first demonstration of multi-GeV laser wakefield acceleration in a fully optically formed plasma waveguide, with an acceleration gradient as high as 25 GeV/m . The guide was formed via self-waveguiding of < 15 J, 45 fs (< ~ 300 TW) pulses over 20 cm in a low-density hydrogen gas jet, with accelerated electron bunches driven up to 5 GeV in quasimonoenergetic peaks of relative energy width as narrow as ~ 15 % , with divergence down to ~ 1mrad and charge up to tens of picocoulombs. Energy gain is inversely correlated with on-axis waveguide density in the range Ne0 = (1.3 – 3.2) x 10 17 cm –3 . We find that shot-to-shot stability of bunch spectra and charge are strongly dependent on the pointing of the injected laser pulse and gas jet uniformity. We also observe evidence of pump depletion-induced dephasing, a consequence of the long optical guiding distance.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

The Effects of Material-Filled Voids on Detonation Wave Shape in Rubberized RDX Explosives

The sensitivity of explosives is affected by inhomogeneities within the material. This is evident in the increased shock sensitivity of explosives with slightly lower densities resulting from an increased number of hotspots. The influence of hotspots on explosive initiation has been well studied; however, few studies have been conducted on the effect of intermediate-sized voids (0.1–10 mm) on a propagating detonation wave. Cylindrical voids filled with air have been studied for diameters ranging from 0.3 mm to 0.8 mm for both 1,3,5,7-tetranitro-1,3,5,7-tetrazocane (HMX) and 1,3,5-trinitro-1,3,5-triazinane (RDX)-based rubberized explosives. Continuing the investigation into single cylindrical voids, this study examined the effects of 0.5 mm diameter voids filled with different inert cylindrical metals on the detonation wave shape for an RDX-based rubberized explosive. The metals selected for experiments were 1066 aluminum, brass, copper, and tungsten. The propagation of the detonation wave was captured using a digital streak camera. Experimental results showed that the extent of detonation wave shaping was closely tied to the density differential between the bulk explosive and metal insert. Forty-four different filler materials, including non-metals, were simulated using a hydrodynamic code to further analyze material inclusion effects. The main factors hypothesized to be of interest were bulk sound speed, shock impedance, and filler material density. We found that the local detonation delay could be correlated fairly well to a ratio of bulk sound speed and density. Understanding the influence of material inclusions on detonation performance and wave shape allows for tailoring of detonations.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗
DOE OSTI2020

A review of the application of 2D isotropic-anisotropic correlation NMR spectroscopy in structural studies of chalcogenide glasses

The application of solid-state high-resolution NMR spectroscopy in the structural investigation of chalcogenide glasses in Ge/As/P/Si-X (X = S, Se,Te) systems has remained challenging even for the spin-1/2 nuclides ( 29 Si, 31 P, 77 Se, 125 Te), owing to their low natural abundance (except for 31 P), slow spin-lattice relaxation rate and large CSA and chemical shift distribution induced line broadening effects. However, most of these deleterious effects can be successfully overcome in two-dimensional (2D) isotropic-anisotropic correlation NMR experiments, especially when performed at high magnetic field and in conjunction with the Car-Purcell-Meiboom-Gill (CPMG) echo train acquisition. Here, we present a short introduction to the basic principles of such experiments and review their applications over the last decade in deciphering various short- and intermediate- range structural characteristics of chalcogenide glasses in S-Se, Se-Te, Ge-Se, As-Se and Si-Se systems as well as in investigating the molecular dynamics in a P-Se supercooled liquid. We anticipate possible future applications of these 2D isotropic-anisotropic correlation NMR experiments, particularly in conjunction with density functional theory-based calculations of NMR chemical shift tensor parameters and additional signal enhancement schemes, in addressing complex structural correlations and distributions in chalcogenide glasses.

2D NMR↗
DOE OSTI2022

Physical mechanisms for the transition from type-III to large ELMs induced by impurity injection on EAST

Transition from type-III to large-amplitude ELMs induced by neon injection has been observed in the EAST tokamak at overlapping q 95 space between large and small ELMs. With neon injection, pedestal density gradient shows a remarkable increase accompanied by some decrease of pedestal electron temperature, and consequently the pressure gradient increases moderately and edge bootstrap current has minimal change. Further experiment demonstrates that the occurrence of large ELMs after neon injection is highly correlated with the change in edge density. Linear peeling-ballooning stability analysis indicates that the large ELM case is more unstable than the type-III ELM case during the ELM transition. A scan of pedestal density gradient in linear stability analysis shows that the direct destabilizing effect of steep pedestal density gradient on peeling-ballooning instabilities via two-fluid effects could also facilitate the transition to large ELMs. In conclusion, these results could provide more insight into the role of pedestal density gradient on pedestal stability and ELM behavior.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Localized Active Space Pair-Density Functional Theory

Accurate quantum chemical methods for the prediction of spin-state energy gaps for strongly correlated systems are computationally expensive and scale poorly with the size of the system. This makes calculations for many experimentally interesting molecules impractical even with abundant computational resources. Previous work has shown that the localized active space (LAS) self-consistent field (SCF) method can be an efficient way to obtain multiconfiguration SCF wave functions of comparable quality to the corresponding complete active space (CAS) ones. To obtain quantitative results, a post-SCF method is needed to estimate the complete correlation energy. One such method is multiconfiguration pair-density functional theory (PDFT), which calculates the energy based on the density and on-top pair density obtained from a multiconfiguration wave function. In this work, we introduce localized-active-space PDFT, which uses a LAS wave function for subsequent PDFT calculations. The method is tested by computing spin-state energies and gaps in conjugated organic molecules and a bimetallic compound and comparing to the corresponding CAS-PDFT values.

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

Machine learning-accelerated path integral molecular dynamics simulations of reactive organic electrolytes

Hydrogen bonded electrolytes that exhibit accelerated proton transport via sequential reactive hops have drawn interest for their promise in clean energy applications. Molecular dynamics simulations of these electrolytes offer the opportunity to uncover microscopic mechanistic details that could be used to design and tune the properties of candidate electrolyte technologies. However, accurately modeling the proton transfer reactions and transport properties that give rise to high charge conductivites in these electrolytes proves computationally challenging because of the need to perform lengthy condensed phase simulations, treating both the electronic and nuclear degrees of freedom quantum mechanically. In this paper, we demonstrate that such a modeling task can be efficiently achieved with the use of density functional theory (DFT)-trained machine learning potentials (MLP) to accelerate path integral molecular dynamics (PIMD) simulations. We highlight the practical utility of this approach by using it to benchmark how closely PIMD simulations employing different DFT exchange–correlation functionals reproduce the composition-dependent densities, diffusion coefficients, and electrical conductivities of mixtures consisting of imidazole and levulinic acid. Even with the speedup afforded by our MLPs, PIMD simulations remain quite expensive. Furthermore, in order to render PIMD more computationally tractable, we introduce and benchmark the accuracy of a ring polymer contraction approach that leverages a computationally efficient short-range MLP to accelerate our PIMD simulations by an additional factor of four.

Chemical bonding↗
DOE OSTI2025

Production of neutron-rich heavy nuclei in deep-inelastic 208 Pb + 208 Pb collisions within the stochastic mean-field theory

In deep-inelastic collisions of heavy nuclei, reaction products with a wide range of mass and charge are produced. Such collisions been considered as a possible way to produce superheavy nuclei, as an alternative to fusion reactions. To provide reliable theoretical predictions, it is desired to develop microscopic approaches that correctly and accurately describe nucleon transfer processes in dissipative collisions of heavy nuclei. The purpose of the present work is (1) to investigate the mechanism of nucleon transfers in dissipative collisions of two heavy nuclei, and (2) to explore possible pathways to produce neutron-rich heavy nuclei, through detailed theoretical analyses of fluctuations and correlations in nucleon transfers in 208 Pb + 208 Pb reactions. Three-dimensional time-dependent Hartree-Fock (TDHF) calculations are performed for the collisions of 208 Pb + 208 Pb at 𝐸 c.m. = 832, 936, and 1040 MeV, using the Skyrme SLy4d energy density functional. To calculate fluctuations and correlations in nucleon transfers, we employ the stochastic mean-field (SMF) theory, and the results are compared with another theoretical framework currently available, the time-dependent random phase approximation (TDRPA). Primary and secondary production cross sections are calculated with the SMF theory combined with a statistical model, GEMINI ++ . Using information of nucleon flow across a neck of colliding nuclei in TDHF calculations, we solve quantal diffusion equations for fluctuations and correlations in nucleon transfers based on the SMF theory. From the SMF calculations, we obtain the time evolution of diffusion coefficients as well as fluctuations and correlations in nucleon transfers for a range of initial orbital angular momenta. We compare the results of the SMF calculations with those of TDRPA, showing that TDRPA tends to predict substantially larger fluctuations and correlations in strongly damped collisions of heavy nuclei, which exhibit complex initial angular momentum dependence, while the SMF results provide almost constant (stable) values. Using the obtained fluctuations and correlations, we calculate primary and secondary production cross sections for the 208 Pb + 208 Pb collisions. From the results, we find that both lighter and heavier reaction products as compared to 208 Pb are produced for a wide region in the 𝑁−𝑍 plane as primary products, thanks to the quantal diffusion mechanism in the dissipative collisions. However, we show that cross sections for production of heavy nuclei with 𝑍 ≳ 90 or 𝑁 ≳ 135 are washed out due to secondary particle evaporation and/or fission processes. On the other hand, we find that there remain sizable cross sections for production of neutron-rich nuclei along 𝑁 = 126 with 𝑍< 82, even after secondary disintegration processes. We demonstrate that the secondary production cross sections depend weakly on incident energies, but lower (higher) energy is slightly preferred for production of nuclei with smaller (larger) atomic numbers as compared to 𝑍 = 82. Here, based on the microscopic SMF calculations, it has been shown that deep-inelastic collisions of heavy nuclei, such as 208 Pb + 208 Pb examined in this study, can be a promising means to produce neutron-rich heavy nuclei along 𝑁=126. Discrepancies between the SMF and TDRPA approaches are left unsolved for future investigations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Software for the frontiers of quantum chemistry: An overview of developments in the Q-Chem 5 package

This article summarizes technical advances contained in the fifth major release of the Q-Chem quantum chemistry program package, covering developments since 2015. A comprehensive library of exchange-correlation functionals, along with a suite of correlated many-body methods, continues to be a hallmark of the Q-Chem software. The many-body methods include novel variants of both coupled-cluster and configuration-interaction approaches along with methods based on the algebraic diagrammatic construction and variational reduced density-matrix methods. Methods highlighted in Q-Chem 5 include a suite of tools for modeling core-level spectroscopy, methods for describing metastable resonances, methods for computing vibronic spectra, the nuclear-electronic orbital method, and several different energy decomposition analysis techniques. High-performance capabilities including multithreaded parallelism and support for calculations on graphics processing units are described. Q-Chem boasts a community of well over 100 active academic developers, and the continuing evolution of the software is supported by an "open teamware" model and an increasingly modular design.

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

Many-Body Benchmark of Electronic Charge and Spin Densities for Li 1–x NiO 2

Accurate benchmarks are particularly important for highly correlated oxides as mean-field approximations often fail to describe the subtle balance of charge transfer and magnetism in these materials with an accuracy comparable to experimental needs. Here we present accurate diffusion Monte Carlo (DMC) results of the electronic charge and spin densities for the tunable highly correlated oxide Li 1–x NiO 2 for x = 0, 1/2, and 1. To enable quantitative comparisons, we introduce a robust density-partitioning scheme, extending Voronoi analysis to assign atomic charges from spatially noisy DMC densities. We then benchmark common approximations used in density functional theory (DFT). Comparison against DMC shows that r 2 SCAN delivers the most balanced performance across charge, spin, and radial density descriptors, nearly reproducing DMC results for LiNiO 2 and apical Ni sites in Li 0.5 NiO 2 . Hybrid functionals (PBE0, SCAN0) perform unexpectedly poorly, and PBE + U + V yields inconsistent trends between charge and spin densities. Therefore, the r 2 SCAN functional minimizes errors relative to DMC while capturing the variable valence of the Ni ion and also retaining the computational efficiency of DFT for large-scale simulations of the tunable structural and electronic phases of Li1−xNiO2. Our study highlights the importance of accurate benchmarking of the fundamental quantities involved in DFT to select appropriate DFT approximations in order to advance the predictive modeling of charge-transfer-driven phenomena in correlated electron systems.

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

Dynamical correlations leading to site and orbital selective Mott insulator transition in hydrogen doped SmNiO 3

Electron doping induces metal -to -insulator transition (MIT) in SmNiO 3 as realized by experiments. While earlier density functional theory (DFT) studies with static correlations fell short of explaining the recent MIT observations at lower hydrogen concentrations, we present a comprehensive computational investigation employing an advanced approach. We combine DFT with dynamical mean field theory (DFT + DMFT) to efficiently analyze the insulating behavior of hydrogen -doped SmNiO 3 . In contrast to previous theoretical works, our calculations predict an insulator transition occurring at a reduced doping level of H:Ni = 0.5:1. Specifically, while the DFT + U method reveals a gap opening between p-to-d orbitals, the DMFT approach highlights a gap opening between d-to-d orbitals. Our findings uncover a selective Mott transition in site and orbital characteristics, with the Ni ions proximate to the doped hydrogen exhibiting Mott -like traits. Notably, DMFT calculations highlight a pronounced dependence on Hund's parameter J, implying the presence of Hundness in the Mott insulator. Finally, this study underscores the necessity of accounting for dynamical correlations to accurately describe the electronic structure of strongly correlated electron-doped rare-earth nickelates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

An Experimental Investigation of Supercritical Methane Injection Characteristics in a CO2 Environment

Abstract Clean energy generation is gaining significant attention from industries, academia, and governments across the globe. The Allam cycle is one such technology that has been under focus due to its efficiency, environmental friendliness, and economics. This is a direct-fired cycle operating at supercritical conditions using carbon dioxide as a working fluid. Fuel or oxidizer jet mixing with CO2 is a vital phenomenon that governs combustion efficiency, and it is not well understood for the Allam cycle conditions. This paper experimentally investigated the jet characteristics of a methane jet injected into a subcritical to supercritical carbon dioxide environment. A wide range of injection pressures and temperatures were targeted between subcritical to supercritical conditions. Unlike previous studies, the current work focused on injecting lower-density (methane) jets into higher-density (carbon dioxide) environments. Schlieren imaging and methane absorption measurements were simultaneously performed with a CMOS high-speed camera and a 3.39 μm infrared laser. Specifically, we looked at the classical injection parameter of jet spreading angle, which was classically established to be mainly a density ratio function. Here, the jet cone angle was obtained from the postprocessed schlieren imaging. The jet cone angle is a critical characteristic parameter that describes the entrainment rate in a jet; thus, it is a crucial parameter in understanding the nature of the jet. The laser measurements were only used as an additional check to confirm the entry time of methane into the chamber filled with carbon dioxide. Notably, this paper makes a detailed comparison between the jet cone angles of jets with a density ratio. The result showed that the classical correlations, such as Abramovich's theory applied to submerged turbulent gas jets developed for low-density ratio jets, were unsuitable for higher-density ratio jets. It was also observed that the divergence angles were dependent not only on density ratio but also on other parameters such as pressure ratios and reduced pressures.

Engineering↗
DOE OSTI2023

Electronic density response of warm dense matter

Matter at extreme temperatures and pressures—commonly known as warm dense matter (WDM)—is ubiquitous throughout our Universe and occurs in astrophysical objects such as giant planet interiors and brown dwarfs. Moreover, WDM is very important for technological applications such as inertial confinement fusion and is realized in the laboratory using different techniques. A particularly important property for the understanding of WDM is given by its electronic density response to an external perturbation. Such response properties are probed in x-ray Thomson scattering (XRTS) experiments and are central for the theoretical description of WDM. In this work, we give an overview of a number of recent developments in this field. To this end, we summarize the relevant theoretical background, covering the regime of linear response theory and nonlinear effects, the fully dynamic response and its static, time-independent limit, and the connection between density response properties and imaginary-time correlation functions (ITCF). In addition, we introduce the most important numerical simulation techniques, including path-integral Monte Carlo simulations and different thermal density functional theory (DFT) approaches. From a practical perspective, we present a variety of simulation results for different density response properties, covering the archetypal model of the uniform electron gas and realistic WDM systems such as hydrogen. Moreover, we show how the concept of ITCFs can be used to infer the temperature from XRTS measurements of arbitrary complex systems without the need for any models or approximations. Finally, we outline a strategy for future developments based on the close interplay between simulations and experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Dark matter from anomaly cancellation at the LHC

We discuss a class of theories that predict a fermionic dark matter candidate from gauge anomaly cancellation. As an explicit example, we study the predictions in theories where the global symmetry associated with baryon number is promoted to a local gauge symmetry. In this context, the symmetry-breaking scale has to be below the multi-TeV scale in order to be in agreement with the cosmological constraints on the dark matter relic density. The new physical “Cucuyo” Higgs boson in the theory has very interesting properties, decaying mainly into two photons in the low mass region, and mainly into dark matter in the intermediate mass region. We study the most important signatures at the Large Hadron Collider, evaluating the experimental bounds. We discuss the correlation between the dark matter relic density, direct detection, and collider constraints. We find that these theories are still viable and are susceptible to being probed in current, and future high-luminosity, running. Published by the American Physical Society 2024

Butterworth, Jon (ORCID:0000000259055394)↗
DOE OSTI2020

DC Hall coefficient of the strongly correlated Hubbard model

The Hall coefficient is related to the effective carrier density and Fermi surface topology in non-interacting and weakly interacting systems. In strongly correlated systems, the relation between the Hall coefficient and single-particle properties is less clear. Clarifying this relation would give insight into the nature of transport in strongly correlated materials that lack well-formed quasiparticles. In this work, we investigate the DC Hall coefficient of the Hubbard model using determinant quantum Monte Carlo in conjunction with a recently developed expansion of magneto-transport coefficients in terms of thermodynamic susceptibilities. At leading order in the expansion, we observe a change of sign in the Hall coefficient as a function of temperature and interaction strength, which we relate to a change in the topology of the apparent Fermi surface. We also combine our Hall coefficient results with optical conductivity values to evaluate the Hall angle, as well as effective mobility and effective mass based on Drude theory of metals.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Scalable learning of potentials to predict time-dependent Hartree–Fock dynamics

We propose a framework to learn the time-dependent Hartree–Fock (TDHF) inter-electronic potential of a molecule from its electron density dynamics. Although the entire TDHF Hamiltonian, including the inter-electronic potential, can be computed from first principles, we use this problem as a testbed to develop strategies that can be applied to learn a priori unknown terms that arise in other methods/approaches to quantum dynamics, e.g., emerging problems such as learning exchange–correlation potentials for time-dependent density functional theory. We develop, train, and test three models of the TDHF inter-electronic potential, each parameterized by a four-index tensor of size up to 60 × 60 × 60 × 60. Two of the models preserve Hermitian symmetry, while one model preserves an eight-fold permutation symmetry that implies Hermitian symmetry. Across seven different molecular systems, we find that accounting for the deeper eight-fold symmetry leads to the best-performing model across three metrics: training efficiency, test set predictive power, and direct comparison of true and learned inter-electronic potentials. All three models, when trained on ensembles of field-free trajectories, generate accurate electron dynamics predictions even in a field-on regime that lies outside the training set. To enable our models to scale to large molecular systems, we derive expressions for Jacobian-vector products that enable iterative, matrix-free training.

97 MATHEMATICS AND COMPUTING↗