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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Recent Advances for Improving the Accuracy, Transferability, and Efficiency of Reactive Force Fields

Reactive force fields provide an affordable model for simulating chemical reactions at a fraction of the cost of quantum mechanical approaches. However, classically accounting for chemical reactivity often comes at the expense of accuracy and transferability, while computational cost is still large relative to nonreactive force fields. Here, we summarize recent efforts for improving the performance of reactive force fields in these three areas with a focus on the ReaxFF theoretical model. To improve accuracy, we describe recent reformulations of charge equilibration schemes to overcome unphysical long-range charge transfer, new ReaxFF models that account for explicit electrons, and corrections for energy conservation issues of the ReaxFF model. To enhance transferability we also highlight new advances to include explicit treatment of electrons in the ReaxFF and hybrid nonreactive/reactive simulations that make it possible to model charge transfer, redox chemistry, and large systems such as reverse micelles within the framework of a reactive force field. To address the computational cost, we review recent work in extended Lagrangian schemes and matrix preconditioners for accelerating the charge equilibration method component of ReaxFF and improvements in its software performance in LAMMPS.

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

Accurate and scalable graph neural network force field and molecular dynamics with direct force architecture

Abstract Recently, machine learning (ML) has been used to address the computational cost that has been limiting ab initio molecular dynamics (AIMD). Here, we present GNNFF, a graph neural network framework to directly predict atomic forces from automatically extracted features of the local atomic environment that are translationally-invariant, but rotationally-covariant to the coordinate of the atoms. We demonstrate that GNNFF not only achieves high performance in terms of force prediction accuracy and computational speed on various materials systems, but also accurately predicts the forces of a large MD system after being trained on forces obtained from a smaller system. Finally, we use our framework to perform an MD simulation of Li 7 P 3 S 11 , a superionic conductor, and show that resulting Li diffusion coefficient is within 14% of that obtained directly from AIMD. The high performance exhibited by GNNFF can be easily generalized to study atomistic level dynamics of other material systems.

Chemistry↗
DOE OSTI2019

Screening Diffusion of Small Molecules in Flexible Zeolitic Imidazolate Frameworks Using a DFT-Parameterized Force Field

Quantitatively modeling adsorbate diffusion through zeolitic imidazolate frameworks (ZIFs) must account for the inherent flexibility of these materials. Here, the lack of a transferable intramolecular ZIF force field (FF) for use in classical simulations has previously made an accurate simulation of adsorbate diffusion in many ZIFs impossible. We resolve this problem by introducing a density functional theory parameterized force field (FF) for ZIFs named the intraZIF-FF, which includes perturbations to the class I force fields previously used to model ZIFs. This FF outperforms ad hoc force fields at predicting ab initio relative energies and atomic forces taken from fully periodic ab initio molecular dynamics simulations of SALEM-2, ZIF-7, ZIF-8, and ZIF-90. We use the intraZIF-FF to predict the infinite dilution self-diffusion coefficients of 30 adsorbates with molecular diameters ranging from 2.66 to 7.0 Å in these 4 ZIFs. These results greatly increase the number of adsorbates for which accurate information about molecular diffusion in ZIFs is available.

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

Bayesian force fields from active learning for simulation of inter-dimensional transformation of stanene

Abstract We present a way to dramatically accelerate Gaussian process models for interatomic force fields based on many-body kernels by mapping both forces and uncertainties onto functions of low-dimensional features. This allows for automated active learning of models combining near-quantum accuracy, built-in uncertainty, and constant cost of evaluation that is comparable to classical analytical models, capable of simulating millions of atoms. Using this approach, we perform large-scale molecular dynamics simulations of the stability of the stanene monolayer. We discover an unusual phase transformation mechanism of 2D stanene, where ripples lead to nucleation of bilayer defects, densification into a disordered multilayer structure, followed by formation of bulk liquid at high temperature or nucleation and growth of the 3D bcc crystal at low temperature. The presented method opens possibilities for rapid development of fast accurate uncertainty-aware models for simulating long-time large-scale dynamics of complex materials.

Chemistry↗
DOE OSTI2020

Equilibrium carbon isotope fractionation factors of hydrocarbons: Semi-empirical force-field method

Here, we have calculated the reduced partition function ratios for carbon isotopes (β-factor) of 67 hydrocarbons (alkanes, alkenes, alkynes, cycloalkanes, and aromatics), including their 267 single-substituted isotopomers. The calculations were performed using the harmonic oscillator – rigid rotator model and the Urey / Bigeleisen-Mayer approach. Normal frequencies of molecular vibrations of the isotopologues were calculated from the molecular structures data and valence field force constants stored in the Light-handled Elucidation of Vibrations (LEV) database elaborated by Dr. Gribov and his colleagues in Russia. The LEV database is constructed from experimental spectroscopic and structural data by solving inverse problems of molecular vibrations. The LEV is internally consistent and the most comprehensive database available to date. The β-factor were calculated in the temperature range of 200–800 K with a 10 K step. Our calculations predict that the β-factors increase with an increasing number of C atoms within the same groups of hydrocarbons (e.g., alkanes). Our calculations also show a general descending order of 13 C enrichments among the different groups of hydrocarbons: cycloalkanes, aromatics, alkenes (double bonds) and isoalkanes, alkanes, alkynes (triple bonds). Position-specific, intramolecular isotope effects within hydrocarbons are determined by the β-factors of C in the different functional groups in the order: quaternary (C), tertiary (methine, CH), secondary (methylene, CH 2 ), primary (methyl, CH 3 ) and double bond (C=C), saturated bond (C - C), triple bond (HC≡). Our calculations on bulk and position-specific carbon isotope β-factors of the hydrocarbons, which are generally consistent with very limited ab initio calculations in the literature, are internally consistent and the most comprehensive to date for future applications to position-specific isotope geochemistry of hydrocarbons.

58 GEOSCIENCES↗
DOE OSTI2019

Time-Dependent Complete Active Space Embedded in Polarizable Force Field

Electron correlation and environmental effects play important roles in electron dynamics and spectroscopic observables of chemical systems in condensed phase. In this paper, we present a time-dependent complete active space configuration interaction (TD-CASCI) approach embedded in a polaraizable force filed, MMPol. The present implementation of TD-CASCI/MMPol utilizes a direct matrix-vector contraction, allowing studies of large systems. This scheme is used to study the solvatochromic shift of coumarin 153 in methanol. The TD-CASCI/MMPol approach captures the double excitation character in the excited state wave function and accurately predicts the solvatochromic red-shift of coumarin 153 dye within the experimental range, outperforming linear response time-dependent density functional theory. The effect of using different reference orbitals for the TD-CASCI/MMPol simulation is also investigated, highlighting the need for an unbiased treatment of all electronic states in the energy range of interest.

Liu, Hongbin↗
DOE OSTI2018

Microscopic Behaviors of Tri-n-Butyl Phosphate, n-Dodecane and Their Mixtures at Air/Liquid and Liquid/Liquid Interfaces: An AMBER Polarizable Force Field Study

In solvent extraction processes for recovering metal ions from used nuclear fuel, as well as other industrial applications, a better understanding of the metal complex phase transfer phenomenon would greatly aid ligand design and process optimization. We have approached this challenge by utilizing classical molecular dynamics simulations technique to gain visual appreciation of the vapor/liquid and liquid/liquid interface between tri-n-butyl phosphate (TBP) and n-dodecane with air and water. In this study, we successfully reparameterized polarizable force fields for TBP and n-dodecane that accurately reproduced several of their thermophysical properties such as: density, heat of vaporization, and dipole moment. Our models were able to predict the surface and interfacial tension of different systems when compared to experimental results also performed by us. Through this study, we gained numerous atomistic understanding of the behaviors of TBP and n-dodecane at the interface against air and water, useful in further computational studies of such systems. Lastly, our studies indicate that the initial configuration of a simulation may have a large effect on the final result.

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

Computational Screening of Cationic Zeolites for n -Butane/Methane Separations Using Quantitatively Accurate First-Principles-Derived Force Fields

We developed force fields for linear alkanes in Na and Ca-exchanged zeolites based on periodic first-principles calculations with coupled cluster corrections. These force fields were validated by comparing the simulated adsorption properties with extensive experimental data. As an example of using these force fields, we screened silica and aluminosilicate zeolites for separation of n-butane/methane mixtures in several different separation processes. A key step in this screening was the use of an interpolation method to create accurate zeolite structures that take account of the lattice constant changes for different Si/Al ratios for a given zeolite topology. We focused on zeolite structures that have known synthesis routes, so the materials selected from our calculations can be tested experimentally. Several promising materials that show good separation performance were selected for more detailed simulations.

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

Using Neural Network Force Fields to Ascertain the Quality of Ab Initio Simulations of Liquid Water

Accurately simulating the properties of bulk water, despite the apparent simplicity of the molecule, is still a challenge. In order to fully understand and reproduce its complex phase diagram, it is necessary to perform simulations at the ab initio level, including quantum mechanical effects both for electrons and nuclei. This comes at a high computational cost, given that the structural and dynamical properties tend to require long timescales and large simulation cells. In this work, we evaluate the errors that density functional theory (DFT)-based simulations routinely incur into due time- and size-scale limitations. These errors are evaluated using neural-network-trained force fields that are accurate at the level of DFT methods. We compare different exchange and correlation potentials for properties of bulk water that require large timescales. Here we show that structural properties are less dependent on the system size and that dynamical properties such as the diffusion coefficient have a strong dependence on the simulation size and timescale. Our results facilitate comparisons of DFT-based simulation results with experiments and offer a path to discriminate between model and convergence errors in these simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2005

Prediction of Mechanical Properties of Polymers With Various Force Fields

The effect of force field type on the predicted elastic properties of a polyimide is examined using a multiscale modeling technique. Molecular Dynamics simulations are used to predict the atomic structure and elastic properties of the polymer by subjecting a representative volume element of the material to bulk and shear finite deformations. The elastic properties of the polyimide are determined using three force fields: AMBER, OPLS-AA, and MM3. The predicted values of Young s modulus and shear modulus of the polyimide are compared with experimental values. The results indicate that the mechanical properties of the polyimide predicted with the OPLS-AA force field most closely matched those from experiment. The results also indicate that while the complexity of the force field does not have a significant effect on the accuracy of predicted properties, small differences in the force constants and the functional form of individual terms in the force fields determine the accuracy of the force field in predicting the elastic properties of the polyimide.

Odegard, Gregory M.↗
DOE OSTI2018

Molecular dynamics simulation of sodium aluminosilicate glass structures and glass surface-water reactions using the reactive force field (ReaxFF)

Reactive potentials are increasingly used to study the properties of glasses and glass water reactions in a reactive molecular dynamics (MD) framework. In this study, we have simulated a ternary sodium aluminosilicate glass and investigated the initial stages of the glass surface-water reactions at 300 K using reactive force field (ReaxFF). On comparison of the simulated glass structures generated using ReaxFF and classical Buckingham potentials, our results show that the atomic density profiles calculated for the surface glass structures indicate a bond-angle distribution dependency. The atomic density profiles also show higher concentrations of non-bridging oxygens (NBOs) and sodium ions at the glass surface. Additionally, we present our results of formation of silanol species and the diffusion of water molecules at the glass surface using ReaxFF.

Chemistry↗
DOE OSTI2020

Liquid to crystal Si growth simulation using machine learning force field

Machine learning force field (ML-FF) has emerged as a potential promising approach to simulate various material phenomena for large systems with ab initio accuracy. However, most ML-FFs have been used to study the phenomena relatively close to the equilibrium ground states. In this work, we have studied a far from equilibrium system of liquid to crystal Si growth using ML-FF. Here, we found that our ML-FF based on ab initio decomposed atomic energy can reproduce all the aspects of ab initio simulated growth, from local energy fluctuations to transition temperatures, to diffusion constant, and growth rates. We have also compared the growth simulation with the Stillinger-Weber classical force field and found significant differences. A procedure is also provided to correct a systematic fitting bias in the ML-FF training process, which exists in all training models, otherwise critical results like transition temperature will be wrong.

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

High-pressure and temperature neural network reactive force field for energetic materials

Reactive force fields for molecular dynamics have enabled a wide range of studies in numerous material classes. These force fields are computationally inexpensive compared with electronic structure calculations and allow for simulations of millions of atoms. However, the accuracy of traditional force fields is limited by their functional forms, preventing continual refinement and improvement. Therefore, we develop a neural network-based reactive interatomic potential for the prediction of the mechanical, thermal, and chemical responses of energetic materials at extreme conditions. The training set is expanded in an automatic iterative approach and consists of various CHNO materials and their reactions under ambient and shock-loading conditions. Further, this new potential shows improved accuracy over the current state-of-the-art force fields for a wide range of properties such as detonation performance, decomposition product formation, and vibrational spectra under ambient and shock-loading conditions.

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

A transferable classical force field to describe glyme based lithium solvate ionic liquids

A non-polarizable force field for lithium (Li + ) and bis(trifluoromethanesulfonyl)imide (TFSI – ) ions solvated in diglyme at around 0.2 mol fraction salt concentration was developed based on ab initio molecular dynamics (AIMD) simulations and a modified polymer consistent force field model. A force–torque matching based scheme, in conjunction with a genetic algorithm, was used to determine the Lennard-Jones (LJ) parameters of the ion–ion and ion–solvent interactions. This force field includes a partial charge scaling factor and a scaling factor for the 1–4 interactions. The resulting force field successfully reproduces the radial distribution function of the AIMD simulations and shows better agreement compared to the unmodified force field. The new force field was then used to simulate salt solutions with glymes of increasing chain lengths and different salt concentrations. The comparison of the MD simulations, using the new force field, with experimental data at different salt concentrations and AIMD simulations on equimolar concentrations of the triglyme system demonstrates the transferability of the force field parameters to longer glymes and higher salt concentrations. Furthermore, the force field appears to reproduce the features of the experimental x-ray structure factors, suggesting accuracy beyond the first solvation shell, for equimolar salt solutions using both triglyme and tetraglyme as the solvent. Altogether, the new force field was found to accurately reproduce the molecular descriptions of LiTFSI-glyme systems not only at various salt concentrations but also with glymes of different chain lengths. Thus, the new force field provides a useful and accurate tool to perform in silico studies of this family of systems at the atomistic level.

25 ENERGY STORAGE↗
NASA NTRS1993

Accurate Quartic Force Fields and Vibrational Frequencies for HCN and HNC

The quartic force fields of HCN and HNC are determined using atomic natural orbital one-particle basis sets of spdf/spd and spdfg/spdf quality in conjunction with the CCSD(T) electron correlation method (singles and doubles coupled-cluster theory plus a perturbational estimate of the effects of connected triple excitations). The HCN force field is in good agreement with a recent experimentally derived force field and also with the force field recently computed by Wong and Bacskay. On the basis of the good agreement obtained for HCN, it is argued that the ab initio quartic force field for HNC is superior to a prior force field derived from experiment. The harmonic frequencies of HNC are predicted to be 3822 +/- 10,472 +/- 5, and 2051 +/-10/cm for omega1, omega2, and omega3, respectively; the experimentally derived values are above these values and fall outside the estimated uncertainties. Using the quartic force field, spectroscopic constants are predicted for HNC based on a vibrational second-order perturbation theory analysis. It is also asserted that the gas-phase fundamental v(sub 3) for HNC is slightly lower than the matrix isolation value. The range of validity of the quartic force fields is investigated by comparison of variational vibrational energies computed with the quartic force fields to those obtained from our recently reported global HCN/HNC potential energy surface and also to experimental data.

Lee, Timothy J.↗