Equation of state predictions for ScF3 and CaZrF6 with neural network-driven molecular dynamics.

In silico property prediction based on density functional theory (DFT) is increasingly performed for crystalline materials. Whether quantitative agreement with experiment can be achieved with current methods is often an unresolved question, and may require detailed examination of physical effects such as electron correlation, reciprocal space sampling, phonon anharmonicity, and nuclear quantum effects (NQE), among others. In this work, we attempt first-principles equation of state prediction for the crystalline materials ScF3 and CaZrF6, which are known to exhibit negative thermal expansion (NTE) over a broad temperature range.

-Heterocyclic Carbene Formation in the Ionic Liquid [EMIM][OAc]: Elucidating Solvation Effects with Reactive Molecular Dynamics Simulations.

Recent experimental and theoretical work has debated whether -heterocyclic carbenes (NHCs) are natively present in imidazolium-based ionic liquids (ILs) such as 1-ethyl-3-methylimidazolium acetate ([EMIM][OAc]) at room temperature. Because NHCs are powerful catalysts, determining their presence within imidazolium-based ILs is important, but experimental characterization is difficult due to the transient nature of the carbene species. Because the carbene formation reaction involves acid-base neutralization of two ions, ion solvation will largely dominate the reaction free energy and thus must be considered in any quantum chemical investigation of the reaction.

Development and Validation of AMBER-FB15-Compatible Force Field Parameters for Phosphorylated Amino Acids.

Phosphorylation of select amino acid residues is one of the most common biological mechanisms for regulating protein structures and functions. While computational modeling can be used to explore the detailed structural changes associated with phosphorylation, most molecular mechanics force fields developed for the simulation of phosphoproteins have been noted to be inconsistent with experimental data. In this work, we parameterize force fields for the phosphorylated forms of the amino acids serine, threonine, and tyrosine using the ForceBalance software package with the goal of improving agreement with experiments for these residues.

Physics-based, neural network force fields for reactive molecular dynamics: Investigation of carbene formation from [EMIM][OAc].

Reactive molecular dynamics simulations enable a detailed understanding of solvent effects on chemical reaction mechanisms and reaction rates. While classical molecular dynamics using reactive force fields allows significantly longer simulation time scales and larger system sizes compared with ab initio molecular dynamics, constructing reactive force fields is a difficult and complex task. In this work, we describe a general approach following the empirical valence bond framework for constructing ab initio reactive force fields for condensed phase simulations by combining physics-based methods with neural networks (PB/NNs).

Proton Transport in [BMIM][BF]/Water Mixtures Near the Percolation Threshold.

The incorporation of ionic liquids into existing proton exchange membrane (PEM) materials has been shown to enhance thermal stability and improve conductivity at reduced water content. Because proton transport is dictated by an interplay between vehicular diffusion and the Grotthuss mechanism, it is expected that the nanoscale structure of the resulting ionic liquid/water networks will sensitively influence transport properties. In this work, we study proton transport in [BMIM][BF]/water mixtures of systematically varying water volume fraction, focusing on concentrations near the percolation threshold in which water networks are connected over macroscopic length scales.

Tuning Water Networks via Ionic Liquid/Water Mixtures.

Water in nanoconfinement is ubiquitous in biological systems and membrane materials, with altered properties that significantly influence the surrounding system. In this work, we show how ionic liquid (IL)/water mixtures can be tuned to create water environments that resemble nanoconfined systems. We utilize molecular dynamics simulations employing force fields to extensively characterize the water structure within five different IL/water mixtures: [BMIM + ][BF 4 - ], [BMIM + ][PF 6 - ], [BMIM + ][OTf - ], [BMIM + ][NO 3 - ]and [BMIM + ][TFSI - ] ILs at varying water fraction.