Many-Body Molecular Dynamics Simulations of Ionic Systems: From Clusters to Bulk and Interfaces

The overarching goal of this research project was to develop an novel theoretical/computational methodology, rigorously derived from a many-body formalism, for modeling ionic systems from the gas to the condensed phase. We achieved this goal by combining data-driven representations of many-body short-range quantum mechanical interactions, which arise from the overlap of the electron densities of individual molecules, with physics-based representations of many-body polarization and long-range interactions. We demonstrated that the resulting many-body potential energy functions display chemical accuracy for each term of the many-body expansion of the interaction energies between ions and water, thus enabling molecular-level computer simulations of ionic systems with unprecedented accuracy and predictive power, from the gas to the condensed phase.