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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

On the computational solution of vector-density based continuum dislocation dynamics models: A comparison of two plastic distortion and stress update algorithms

Continuum dislocation dynamics models of mesoscale plasticity consist of dislocation transport-reaction equations coupled with crystal mechanics equations. The coupling between these two sets of equations is such that dislocation transport gives rise to the evolution of plastic distortion (strain), while the evolution of the latter fixes the stress from which the dislocation velocity field is found via a mobility law. Earlier solutions of these equations employed a staggered solution scheme for the two sets of equations in which the plastic distortion was updated via time integration of its rate, as found from Orowan's law. In this work, we show that such a direct time integration scheme can suffer from accumulation of numerical errors. We introduce an alternative scheme based on field dislocation mechanics that ensures consistency between the plastic distortion and the dislocation content in the crystal. The new scheme is based on calculating the compatible and incompatible parts of the plastic distortion separately, and the incompatible part is calculated from the current dislocation density field. Stress field and dislocation transport calculations were implemented within a finite element based discretization of the governing equations, with the crystal mechanics part solved by a conventional Galerkin method and the dislocation transport equations by the least squares method. A simple test was first performed to show the accuracy of the two schemes for updating the plastic distortion, which shows that the solution method based on field dislocation mechanics is more accurate. This method then was used to simulate an austenitic steel crystal under uniaxial loading and multiple slip conditions. By considering dislocation interactions caused by junctions, a hardening rate similar to discrete dislocation dynamics simulation results was obtained. Finally, the simulations show that dislocations exhibit some self-organized structures as the strain is increased.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Influence of surface chemistry on Li nucleation energetics on graphene-based surfaces

Lithium metal is a promising high-capacity anode material for solid-state batteries, but it typically suffers from poor cyclability. Carbon scaffold hosts have the potential to improve this performance due to their high electronic conductivity and large surface area, which facilitates lithium-ion adsorption and desorption. Scaffold surface chemistry is known to significantly influence performance outcomes, but the details of these interactions are not fully understood. Here, this study employs first-principles simulations to explore lithium transport and nucleation on graphene anodes with various surface chemistries. Using enhanced sampling techniques, ab initio molecular dynamics, and density functional theory calculations, we find that although surface chemistry has a minimal impact on lithium interfacial transport, it influences surface nucleation significantly. Both heteroatom dopants and intrinsic defects lower the nucleation barrier, creating a more favorable environment for lithium nucleation compared to pristine graphene. In addition, our results reveal a complex interplay between surface lithium concentration, lithium transport, and nucleation kinetics. These findings highlight the potential of surface modifications to precisely control nucleation processes on carbon-based anodes and provide design guidance for reducing dendrite formation and improving the cycle life of solid-state batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Runaway electron beam dynamics at low plasma density in DIII-D: energy distribution, current profile, and internal instability

Parameters of the post-disruption runaway electron (RE) beam in the collisionless background plasma achieved after deuterium injection are investigated in DIII-D. The spatially resolved RE energy distribution function is measured for the first time during the RE plateau stage by inverting hard X-ray bremsstrahlung spectra. It has maximum energy up to 20 MeV and a non-monotonous feature at 5{6 MeV observed only in the core of the beam supporting the possibility of kinetic instabilities. The RE current profile is reconstructed for the first time using the spatially resolved RE energy distribution. It is found to be more peaked than the pre-disruption plasma current, with higher internal inductance, suggesting preferential formation of REs in the core plasma or potentially a radially inward motion of the REs. The accessed relatively low-current (180 kA) RE beam is found stable, likely due to its elevated q profile. From this base stable equilibrium, instability is accessed by ramping the solenoid current. Under a large applied accelerating loop voltage an internal kink mode is observed. The kink mode leads to sawtooth-like relaxation of the RE current profile, but drives no RE loss. Under conditions of a large decelerating voltage, chirping Alfvénic instabilities driven by REs during the RE plateau stage are observed for the first time. The low-frequency (0.1{7 MHz) Alfvénic instabilities, supposedly compressional Alfvén eigenmodes, are found to be correlated with a RE loss signal. Finally, this provides novel plasma conditions to study these instabilities and investigate opportunities to utilize them for RE control. Bifurcated electron cyclotron emission (ECE) spectrum is measured during the collisionless RE plateau, with a break point at ≈100 GHz suggesting resonant absorption of the ECE at low frequencies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Onset of anharmonicity and thermal conductivity in SnSe

The anharmonicity in SnSe is investigated through the analysis of moments of 119Sn nuclear resonant inelastic x-ray scattering and ab initio molecular dynamics calculations. Experimental evidences show that the anharmonic behavior started around 300 K, substantially lower than the usually suggested structural transition at 800 K. Both theory and experiments reveal substantial lifetime broadening and frequency renormalization of the optical phonons. Additionally, thermal conductivities calculated from the temporal energy moment using the Einstein diffusion equation are in good agreement with previous experiments. The abrupt increase of the thermal power near 800 K is driven by an electronic factor and not by the enhanced anharmonicity due to structural change.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Understanding Solid-Electrolyte Interphase Formation at the Lithium Metal Anode of Lithium-Sulfur Batteries

Lithium-sulfur (Li-S) batteries are one of the most promising chemistries for the next generation of energy storage devices. In a standard Li-S cell, the metallic lithium anode is an essential component of the battery due to its low density, extremely high theoretical specific capacity, and very low negative electrochemical potential. However, several challenges related to the use of Li metal have prevented this battery technology from becoming commercially available. For instance, Li-anodes are highly reactive, which results in the continuous decomposition of the electrolyte and the formation of the solid-electrolyte interphase (SEI) layer. This, combined with the non-uniform deposition of Liions during plating at the anode surface, can seriously affect the performance, cycling, and safety of the battery. In addition, it has been suggested that a controlled SEI formation at the metallic Li anode can yield enhanced battery performance. Hence, a comprehensive understanding of how the SEI layer is formed can help elucidate improvements in this battery technology. In this work, the formation of the SEI layer in Li-S batteries is investigated using density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. The stability of liquid organic-based electrolyte components, salt concentration, electron-rich environments, and the use of inorganic solid-state electrolyte (SSE) materials are explored in order to provide molecular-level fundamental insights into how the nature and composition of the electrolyte can alter the initial stages of the SEI formation. The products of electrolyte decomposition and electro-/chemical reaction pathways of liquid electrolyte component such as solvent and salts are predicted from AIMD simulations of electrolyte-anode interfaces. Energetics of reactions from DFT ground-state optimizations are also presented to confirm the decomposition mechanisms. Some significant differences are then drawn regarding the use of low and high salt concentrations. Simulations under electron-rich environments show additional multielectron electrochemical reactions of solvent and salt decomposition taking place due to the excess of electrons and the presence of radical anions in the solution. Finally, the initial stages of formation, stability, and main constituents of interfaces between Li-metal and Sbased electrodes with sulfide-based SSEs are characterized in detail.

25 ENERGY STORAGE↗
DOE OSTI2022

Nonadiabatic Molecular Dynamics by Multiconfiguration Pair-Density Functional Theory

Herein, we present the first implementation of multiconfiguration pair-density functional theory (MC-PDFT) ab initio molecular dynamics. MC-PDFT is a multireference electronic structure method that in many cases has a similar accuracy (or even better accuracy) the complete active space second-order perturbation theory (CASPT2) at a significantly lower computational cost. In this study, we introduced MC-PDFT analytical gradients into the SHARC molecular dynamics program for ab initio, nonadiabatic molecular dynamics simulations. We verify our implementation by examining the intersystem crossing dynamics of thioformaldehyde, and we observe excellent agreement with recent CASPT2 and experimental findings. Moreover, with MC-PDFT, we could perform dynamics simulations with the 12 electron in 10 orbitals active space that was computationally too expensive for direct dynamics with CASPT2.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Multi-site reaction dynamics through multi-fragment density matrix embedding

The practical description of disordered chemical reactions, where the reactions involve multiple species at multiple sites, is presently a challenge using correlated electronic structure methods due to their high computational cost and steep scaling. Here, we describe the gradient theory of multi-fragment density matrix embedding theory, which potentially provides a minimal computational framework to model such processes at the correlated electron level. We present the derivation and implementation of the gradient theory, its validation on model systems and chemical reactions using density matrix embedding, and its application to a molecular dynamics simulation of proton transport in a small water cluster, a simple example of multi-site reaction dynamics.

Chemistry↗
DOE OSTI2023

Dynamic Structure of Magnetized High Energy Density Plasmas (Final Report)

This report summarizes results of project DE-SC0022202 ``Dynamic Structure of Magnetized High Energy Density Plasmas,'' which was originally funded for the period 08/01/2021 - 7/31/2022, but was no-cost extended to 7/31/2023. The primary objectives of the work, as stated in the original proposal, were ``develop a theory to describe a novel state of magnetized high energy density plasmas, benchmark the theory using first-principles molecular dynamics simulations, and apply the results to develop a means to interpret x-ray scattering measurements in future experiments.'' These were the goals of the original project proposal, which was for a 3 year project. The project was ultimately funded for 1 year, and so the work completed focused on the goals described for only the first year of the proposed work. This included further developing a kinetic theory for strongly magnetized plasmas, applying it to compute fluid-scale (MHD) transport coefficients, and to test the predictions using molecular dynamics simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Extended Lagrangian Born–Oppenheimer molecular dynamics for orbital-free density-functional theory and polarizable charge equilibration models

We report extended Lagrangian Born–Oppenheimer molecular dynamics (XL-BOMD) is formulated for orbital-free Hohenberg–Kohn density-functional theory and for charge equilibration and polarizable force-field models that can be derived from the same orbital-free framework. The purpose is to introduce the most recent features of orbital-based XL-BOMD to molecular dynamics simulations based on charge equilibration and polarizable force-field models. These features include a metric tensor generalization of the extended harmonic potential, preconditioners, and the ability to use only a single Coulomb summation to determine the fully equilibrated charges and the interatomic forces in each time step for the shadow Born–Oppenheimer potential energy surface. The orbital-free formulation has a charge-dependent, short-range energy term that is separate from long-range Coulomb interactions. This enables local parameterizations of the short-range energy term, while the long-range electrostatic interactions can be treated separately. The theory is illustrated for molecular dynamics simulations of an atomistic system described by a charge equilibration model with periodic boundary conditions. The system of linear equations that determines the equilibrated charges and the forces is diagonal, and only a single Ewald summation is needed in each time step. The simulations exhibit the same features in accuracy, convergence, and stability as are expected from orbital-based XL-BOMD.

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

Enhancing the efficiency of time-dependent density functional theory calculations of dynamic response properties

X-ray Thomson scattering (XRTS) constitutes an essential technique for diagnosing material properties under extreme conditions, such as high pressures and intense laser heating. Time-dependent density functional theory (TDDFT) is one of the most accurate available ab initio methods for modeling XRTS spectra, as well as a host of other dynamic material properties. However, strong thermal excitations, along with the need to account for variations in temperature and density as well as the finite size of the detector significantly increase the computational cost of TDDFT simulations compared to ambient conditions. In this work, we present a broadly applicable method for optimizing and enhancing the efficiency of TDDFT calculations. Our approach is based on a one-to-one mapping between the dynamic structure factor and the imaginary time density–density correlation function, which naturally emerges in Feynman’s path integral formulation of quantum many-body theory. Specifically, we combine rigorous convergence tests in the imaginary time domain with a constraints-based attenuation of narrow-band fluctuations to improve the efficiency of TDDFT modeling without the introduction of any significant bias. As a result, we can report a speed-up by up to an order of magnitude, thus substantially reducing the burden of computational cost required for XRTS analysis.

Moldabekov, Zhandos A. [Helmholtz-Zentrum Dresden-↗
DOE OSTI2022

Identification of efficient and stable solid-solid electrochemical interfaces for Li-S batteries. Final Report

The objective of this work is to develop a better understanding of the interactions between battery components that drive the observed battery performance. Using computational tools at the atomistic level, we elucidate molecular, crystal, and amorphous structures, interfacial structures and reactions, and electrochemical behavior. We focus on Li metal anodes, liquid electrolytes, solid electrolytes, S cathodes, and metal-oxide cathodes, and their corresponding interfaces. Within liquid electrolytes, we study their bulk structure and dynamics, as a function of salt concentration. The analysis allows to understand the formation of localized high concentrated regions as the solvent is substituted by a weakly interacting diluent species. Analysis of the electron distribution yields the reactive behavior at interfaces. Moreover, we employ tools that allow the characterization of ion and electron transport at interfaces, during the processes of solvation and desolvation occurring while cycling. For Sulfur cathodes we elucidate synthesis processes and the role of carbon-sulfur and nitrogen-sulfur interactions not only to provide electronic conductivity but also to define alternative reaction pathways during discharge of Li-S batteries. Full-cell simulations offer new insights regarding the integration of all the battery components. Our studies also include solid electrolytes and their interfaces with Li metal, S-C, and metal-oxide electrodes.

25 ENERGY STORAGE↗
DOE OSTI2024

Orbital-selective time-domain signature of nematicity dynamics in the charge-density-wave phase of La 1.65 Eu 0.2 Sr 0.15 CuO 4

Understanding the interplay between charge, nematic, and structural ordering tendencies in cuprate superconductors is critical to unraveling their complex phase diagram. Using pump–probe time-resolved resonant X-ray scattering on the (0 0 1) Bragg peak at the Cu L 3 and O K resonances, we investigate nonequilibrium dynamics of Q a = Q b = 0 nematic order and its association with both charge density wave (CDW) order and lattice dynamics in La 1.65 Eu 0.2 Sr 0.15 CuO 4 . The orbital selectivity of the resonant X-ray scattering cross-section allows nematicity dynamics associated with the planar O 2 p and Cu 3 d states to be distinguished from the response of anisotropic lattice distortions. A direct time-domain comparison of CDW translational-symmetry breaking and nematic rotational-symmetry breaking reveals that these broken symmetries remain closely linked in the photoexcited state, consistent with the stability of CDW topological defects in the investigated pump fluence regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Probability Density Function Control for Stochastic Nonlinear Systems using Monte Carlo Simulation

This paper presents a fast implementation framework of output probability density function (PDF) control for a class of stochastic nonlinear systems which are subjected to non-Gaussian noises. The statistical properties of the system outputs can be adjusted by shaping the dynamic output probability density function to track the reference stochastic distribution. However, the dynamic probability density function evolution is very difficult to obtain analytically even if the system model and the stochastic distributions of the noises are known. Motivated by Monte Carlo simulation, the dynamic probability density function can be estimated by sampling data which forms the contribution of this paper. In particular, the sampling points are generated following the stochastic distribution of the noise for each instant. These points go through the system would generate the histogram for system outputs, then the dynamic model can be established based on the dynamic histogram which reflects the randomness and the nonlinear dynamics of the investigated system. Based on the established model, the output probability density function tracking can be achieved and the simulation results and discussions show the effectiveness and benefits of the presented framework.

Zhang, Qichun↗
DOE OSTI2021

Confinement effects on the solvation structure of solvated alkaline metal cations in a single-digit 1T-MoS 2 nanochannel: A first-principles study

Confinement plays an important role in determining ion transport in porous materials, which, in turn, may influence the performance of many energy storage and desalination devices. In this work, we combined density functional theory (DFT) with an implicit solvation model and ab initio molecular dynamics (AIMD) to investigate the effects of nanoconfinement on several solvated alkaline metal cations in a single-digit 1T-MoS 2 nanochannel. Our DFT calculations with a solvation model indicated that cations with stronger hydration energy introduce a higher number of co-intercalated water molecules into the channel, consistent with early experimental observation obtained for MXene (2D transition metal carbide) channels. The predicted optimal water numbers for the cations were then used for AIMD simulations that explicitly include the effects of the solvent. When compared with the cations in bulk solution, our simulations showed that the hydration structure and coordination number (CN) of the solvated cations confined in the MoS 2 channel can be significantly altered. Further, we found that larger cations with weaker hydration energy (K + , Rb + , and Cs + ) exhibited a distinctive CN decrease under confinement, while smaller cations (Li + and Na + ) retained a similar hydration shell as in the bulk solution. More specifically, the hydration shell of large cations (K + , Rb + , and Cs + ) in MoS 2 showed similar features of the coordination angle to the bulk, which suggests the partially broken hydration shell with no geometry change under confinement. Our simulations provided insights into the change of the hydration structure of alkaline metal cations under confinement, which may have important implications on their transport in the 1T-MoS 2 channel.

36 MATERIALS SCIENCE↗