Next-Generation Accurate, Transferable, and Polarizable Potentials for Material Simulations.

PHAHST (potentials with high accuracy, high speed, and transferability) intermolecular potential energy functions have been developed from first principles for H2, N2, the noble gases, and a metal-organic material, HKUST-1. The potentials are designed from the outset to be transferable to heterogeneous environments including porous materials, interfaces, and material simulations. This is accomplished by theoretically justified choices for all functional forms, parameters, and mixing rules, including explicit polarization in every environment and fitting to high quality electronic structure calculations using methods that are tractable for real systems. The models have been validated in neat systems by comparison to second virial coefficients and bulk pressure-density isotherms. For inhomogeneous applications, our main target, comparisons are presented to previously published experimental studies on the metal-organic material HKUST-1 including adsorption, isosteric heats of adsorption, binding site locations, and binding site energies. A systematic prescription is provided for developing compatible potentials for additional small molecules and materials. The resulting models are recommended for use in complex heterogeneous simulations where existing potentials may be inadequate.