Two of the most challenging problems at the intersection of electronic structure theory and molecular dynamics simulations are the accurate representation of intermolecular interactions and the development of efficient algorithms applicable to large systems. To some extent, these two problems are antithetical, since accurate calculations of molecular interactions typically require correlated electronic structure methods that are computationally too expensive for applications to large systems. We will describe our many-body molecular dynamics (MB-MD) methodology which overcomes these limitations and enables computer simulations from the gas to the condensed phase, with chemical and spectroscopic accuracy. MB-MD is a unified molecular dynamics framework that integrates data-driven many-body representations derived entirely from correlated electronic structure data with classical and quantum dynamics approaches that allow for a correct description of the molecular motion. We will illustrate the accuracy and predictive ability of our MB-MD methodology in the context of molecular modeling of various aqueous systems in the gas phase, in the bulk, at interfaces, and in metal-organic frameworks, with a particular focus on the relationships between structural and dynamical properties and vibrational spectra.

Data-driven many-body molecular dynamics: Predictive simulations from the gas to the condensed phase

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ACS Fall 2022

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