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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 37 records · Page 2

A foundation model for atomistic materials chemistry

Atomistic simulations of matter, especially those that leverage first-principles (ab initio) electronic structure theory, provide a microscopic view of the world, underpinning much of our understanding of chemistry and materials science. Over the last decade or so, machine-learned force fields have transformed atomistic modeling by enabling simulations of ab initio quality over unprecedented time and length scales. However, early machine-learning (ML) force fields have largely been limited by (i) the substantial computational and human effort required to develop and validate potentials for each particular system of interest and (ii) a general lack of transferability from one chemical system to the next. Here, we show that it is possible to create a general-purpose atomistic ML model, trained on a public dataset of moderate size, that is capable of running stable molecular dynamics for a wide range of molecules and materials. We demonstrate the power of the MACE-MP-0 model-and its qualitative and at times quantitative accuracy-on a diverse set of problems in the physical sciences, including properties of solids, liquids, gases, chemical reactions, interfaces, and even the dynamics of a small protein. The model can be applied out of the box as a starting or "foundation" model for any atomistic system of interest and, when desired, can be fine-tuned on just a handful of application-specific data points to reach ab initio accuracy. Establishing that a stable force-field model can cover almost all materials changes atomistic modeling in a fundamental way: experienced users obtain reliable results much faster, and beginners face a lower barrier to entry. Foundation models thus represent a step toward democratizing the revolution in atomic-scale modeling that has been brought about by ML force fields.

Batatia, Ilyes↗

Modeling prebiotic chemistries with quantum accuracy at classical costs

Molecular Dynamics (MD) simulations using classical force-fields are commonly employed in numerous scientific investigations. However, many natural processes involve bond breaking and quantum forces. This complexity is compounded by the presence of multiple competing length and timescales. For example, accurately modeling the thermodynamics and dynamics of a chemical reaction requires accounting for the concerted movements of numerous solvent molecules and ions with their own fast or slow timescales. While widely used static Density Functional Theory (DFT) calculations at 0 temperature can be beneficial for such investigations, they do not account for dynamics, and lack precision in describing the molecular environments. They particularly fail at correct, rigorous treatments of finite-temperature fluctuations, and thus generalization to experimentally relevant conditions. In PNAS Benayad et al develop a scalable, generalizable approach for designing Neural Network Potentials (NNPs) that can handle chemical reactivity in solvated systems with quantum accuracy at classical costs. Specifically, they study phosphoester bond formation and rupture, which is fundamentally relevant to the Phosphorus-Oxygen bond formation central to life, and especially for the RNA world hypothesis. The framework developed here has the potential to generalize to different chemical reactions of energy and biological relevance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Low-frequency Raman active modes of twisted bilayer MoS 2

Abstract We study the low-frequency Raman active modes of twisted bilayer MoS 2 for several twist angles using a force-field approach and a parametrized bond polarizability model. We show that twist angles near high-symmetry stacking configurations exhibit stacking frustration that leads to significant buckling of the moiré superlattice. We find that atomic relaxation due to the twist is of prime importance. The periodic displacement of the Mo atoms shows the realization of a soliton network, and in turn, leads to the emergence of a number of frequency modes not seen in the high-symmetry stacking systems. Some of the modes are only seen in the XZ Raman polarization setup while others are seen in the XY setup. The symmetry of the normal modes, and how this affects the Raman tensors is examined in detail.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ferroelectric phase transition in group-IV monochalcogenides from an equivariant machine learned force field

Group-IV monochalcogenides are a class of layered ferroelectric semiconductors that have demonstrated spontaneous intrinsic polarization above room temperature. Here, in this study, we use the multi-atomic cluster expansion (MACE) machine learning architecture to train and test a force field capable of modeling the structural properties and second-order ferroelectric-to-paraelectric phase transition in a Group-IV monochalcogenide, GeSe. The model captures the double-well potential energy surface associated with the onset of macroscopic polarization in bulk GeSe within 12.5 meV/atom, as well as near-equilibrium properties like the phonon dispersion. The development of this quantitatively accurate force field enables long-time molecular dynamics simulations, which predict the critical temperature of the ferroelectric-to-paraelectric phase transition in bulk GeSe to be T c = 600 K. This study demonstrates the capabilities of equivariant force-fields to accurately describe phenomena associated with structural symmetry breaking.

ferroelectricity↗

Theories of homogeneous and electrochemical electron transfer in complex media and interfaces (Final Technical Report)

This project makes the next step in establishing practical theories of charge transfer in complex media. The development of formal models is supported by extensive atomistic simulations, quantum calculations of force-field parameters, and direct measurements of charge-transfer spectra. All theory development is supported by experiment, extensive numerical simulations, and through external collaborations.

14 SOLAR ENERGY↗

Wettability of Two-Dimensional Carbon Allotropes from Molecular Simulations

Force-field Monte Carlo and Molecular Dynamics simulations are used to compare wetting behaviors of model carbon sheets mimicking neat graphene, its saturated derivative, graphane, and related planar allotropes penta-graphene, γ-graphyne, and ψ-graphene in contact with aqueous droplets or an aqueous film confined between parallel carbon sheets. Atomistic and area-integrated surface/water potentials are found to be essentially equivalent in capturing moderate differences between the wetting free energies of tested substrates. Despite notable differences in mechanical and electric properties of distinct allotropes, the predicted allotrope/water contact angles span a narrow window of weakly hydrophilic values. Contact angles in the range of 80 ± 10° indicate modest hydration repulsion incapable of competing with van der Waals attraction between carbon particles. Poor dispersibility in neat water is hence a common feature of studied materials.

Biochemistry & Molecular Biology↗

Interplanetary Trajectory Optimization with Powerlimited Propulsion Systems

A trajectory-optimization process is described in which the optimum­ thrust equations are derived using the calculus of variations. The mag­nitude of the thrust is constrained within an upper and a lower bound, but the thrust direction is arbitrary. This formulation allows both the constant-thrust program and the variable-thrust program to be con­sidered. For the constant-thrust program, certain propulsion-system parameters are optimized for maximum final vehicle mass. This theory has been used to study interplanetary missions to Venus and Mars using a power-limited propulsion system. Both one-way and round­ trip rendezvous trajectories are considered. The analysis employs a two-body inverse-square force-field model of three dimensions. An iterative routine used to solve the two-point boundary-value problem is described in the Appendix.

TRAJECTORY↗

Galactic cosmic ray modulation from 1965-1970.

Numerical solutions of the cosmic-ray equation of transport within the solar cavity and including the effects of diffusion, convection, and energy losses due to adiabatic deceleration, have been used to reproduce the modulation of galactic electrons, protons, and helium nuclei observed during the period from 1965 to 1970. Kinetic energies between 10 and 10,000 MeV/nucleon are considered. Computed and observed spectra are given for the years 1965, 1968, 1969, and 1970 together with the diffusion coefficients. These diffusion coefficients are assumed to be of separable form in rigidity and radial dependence, and are consistent with the available magnetic-field power spectra. The force-field solutions are given for these diffusion coefficients and galactic spectra and are compared with the numerical solutions. It is shown that the energy losses and convection lead to near-earth nuclei spectra at kinetic energies less than or equal to 100 MeV/nucleon in which the differential intensity is proportional to the kinetic energy with little dependence on the form of the galactic spectrum. This dependence is in agreement with the observed spectra of all species of atomic nuclei and it is argued that this provides strong observational evidence for the presence of energy losses in the propagation process, and for the exclusion of low-energy galactic nuclei from near earth.

Urch, I. H.↗

Particle distribution functions in modulation theory

Development of a simple formulation of the cosmic ray modulation problem which involves the use of the omnidirectional part of the distribution function in phase space, and the magnitude of the momentum or the rigidity. It is shown that, by employing the proposed formulation, the Compton-Getting factor is greatly simplified, and the well-known force-field equation is reduced to a one-dimensional Vlasov equation. In addition, another Vlasov equation can be written for the very low energy galactic particles which are convected by the solar wind.

Forman, M. A.↗

Analytic approximations in the study of the solar modulation of electrons

Numerical solutions to the transport equation of galactic cosmic rays in the interplanetary medium have been used to investigate the applicability of commonly used approximate analytic solutions for electrons (10 MeV to 10 GeV). We find that for a given cosmic-ray diffusion coefficient the force-field approximation is in reasonable agreement with the numerical solution at energies above 200 MeV, but deviates significantly at lower energies, depending on the shape of the interstellar electron spectrum. The diffusion-convection approximation agrees generally with the numerical solution within a factor of 2 over the entire energy range.

Cummings, A. C.↗

Cosmic ray variations and magnetic field fluctuations in the outer heliosphere

It is formally confirmed that Galactic-cosmic-ray intensity variations measured by Voyager 2 during recovery from solar maximum are caused by traveling compressions and rarefactions in the mean interplanetary magnetic field. Voyager magnetic-field data are used as input to a time-independent, spherically symmetric, cosmic-ray-transport equation in the force-field approximation. The solutions closely followed the count rate of cosmic rays greater than 75 MeV/nucleon over 4 years, during the recovery phase of the 11-year solar-driven cosmic-ray cycle. This strongly supports prior theoretical assertions that turbulent interaction regions traveling with the solar wind are the major cause of the solar-cycle variation of Galactic cosmic rays in the ecliptic region.

Perko, J. S.↗

Solar modulation of galactic antiprotons

Galactic antiproton data of current interest lie in an energy regime heavily influenced by solar modulation. Correcting for it needs to be done more carefully than it has been in the past. The well-known force-field analytic approximation of the spherically-symmetric, steady-state, cosmic-ray transport equation is applied in order to account for modulation down to at least 100 MeV. A sample solution which applies to the currently available antiproton data set (1979-80), and can be used to accurately modulate any possible interstellar antiproton spectrum, is given. The solution is easily adapted for comparison to future measurements. It also shows that boosting the low-energy (less than 600 MeV) side of the interstellar antiproton spectrum will not affect the low-energy spectrum at 1 AU, due to strong adiabatic deceleration during that time.

Perko, J. S.↗

Intensity variations in the interplanetary magnetic field measured by Voyager 2 and the 11-year solar cycle modulation of galactic cosmic rays

New evidence is presented to support the hypothesis that the 11-yr solar cycle modulation of galactic cosmic rays is caused by strong diffusion inside long-lived merged interaction regions. To test this hypothesis, the 1D force-field approximation of the cosmic ray modulation equation is solved. It is assumed that a constant solar wind speed convects magnetic field compressions and rarefactions unchanged through a model heliosphere. The result is a reasonable simulation of the integrated high-energy cosmic ray intensity profile from about 1982 to mid-1989. This period encompasses both the full recovery portion of the last profile from about 1982 to mid-1989. This model responds to the Voyager 2 magnetic field data by correctly timing the beginning of the new modulation cycle in late 1987. It is concluded that the present hypothesis is consistent with the results of this simulation.

Perko, J. S.↗

Cosmic-ray variations and magnetic field fluctuations in the outer heliosphere

We have formally confirmed that galactic cosmic ray intensity variations measured by Voyager 2 during recovery from solar maximum are caused by travelling compressions and rarefactions in the mean interplanetary magnetic field. We used Voyager's nearly continuous magnetic field data as input to a time-independent, spherically-symmetric, cosmic ray transport equation in the force-field approximation. The solutions closely followed the count rate of cosmic rays greater than 75 MeV/nucleon over four years. This strongly supports prior theoretical assertions that turbulent interaction regions travelling with the solar wind are the major cause of the solar-cycle variation of galactic cosmic rays in the ecliptic region.

Perko, J. S.↗

Effects of Structural Deformation and Tube Chirality on Electronic Conductance of Carbon Nanotubes

A combination of large scale classical force-field (UFF), density functional theory (DFT), and tight-binding Green's function transport calculations is used to study the electronic properties of carbon nanotubes under the twist, bending, and atomic force microscope (AFM)-tip deformation. We found that in agreement with experiment a significant change in electronic conductance can be induced by AFM-tip deformation of metallic zigzag tubes and by twist deformation of armchair tubes. The effect is explained in terms of bandstructure change under deformation.

Svizhenko, Alexei↗

Development and assessment of hierarchical multi-reward reinforcement learning based potential for silicene with state-of-the-art models

We develop a new interatomic force field for Silicene, a 2D material with a buckled hexagonal lattice structure with high polymorphism. We introduce new parameterizations of a Tersoff model using a hierarchical multi-reward reinforcement learning (RL) methodology coupled with a continuous Monte Carlo Tree Search optimization. Our model significantly outperforms existing methods by enhancing the accuracy of predictions for the structural and thermodynamic properties of seven silicene polymorphs-including structure, energy, equation of state, elasticity, and phonon dispersion-when compared to established models. We further make a comprehensive comparison of the various models in predicting the mechanical and thermal properties of silicene. We trace the origin of the improved performance to the description of the angular dependence in the bond-order term, suggesting that modifying the angular terms in short-range models is essential to capture the structural diversity in low dimensional systems.

2D materials↗

Accurate determination of solvation free energies of neutral organic compounds from first principles

The main goal of molecular simulation is to accurately predict experimental observables of molecular systems. Another long-standing goal is to devise models for arbitrary neutral organic molecules with little or no reliance on experimental data. While separately these goals have been met to various degrees, for an arbitrary system of molecules they have not been achieved simultaneously. For biophysical ensembles that exist at room temperature and pressure, and where the entropic contributions are on par with interaction strengths, it is the free energies that are both most important and most difficult to predict. We compute the free energies of solvation for a diverse set of neutral organic compounds using a polarizable force field fitted entirely to ab initio calculations. The mean absolute errors (MAE) of hydration, cyclohexane solvation, and corresponding partition coefficients are 0.2 kcal/mol, 0.3 kcal/mol and 0.22 log units, i.e. within chemical accuracy. The model (ARROW FF) is multipolar, polarizable, and its accompanying simulation stack includes nuclear quantum effects (NQE). The simulation tools’ computational efficiency is on a par with current state-of-the-art packages. The construction of a wide-coverage molecular modelling toolset from first principles, together with its excellent predictive ability in the liquid phase is a major advance in biomolecular simulation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗