A General Nonbonded Force Field Based on Accurate Quantum Mechanics Calculations for Elements H-La and Hf-Rn.

Abstract

Noncovalent interactions (NCI) play a central role in numerous physical, chemical, and biological phenomena. An accurate description of NCI is the key to success for any theoretical study in such areas. Although quantum mechanics (QM) methods such as dispersion-corrected density functional theory are sufficiently accurate, their applications are practical only for <300 atoms and <100 ps of simulation time. Thus, empirical force fields (FF) have generally been the only choice for systems with thousands to millions of atoms and for nanoseconds and longer. We want to develop a FF that can be applied to applications of thousands to millions of atoms with an accuracy comparable to QM methods. As the first step, we develop here a new general nonbonded potential (GNB) based on a novel functional form with four adjustable parameters for each element. We report here parameters for elements H-La, Hf-Rn (excluding lanthanides and actinides) by fitting the interaction energy of molecular complexes to QM calculations using the accurate Head-Gordon ωB97M-V density functional. We performed extensive testing of GNB for organic molecules, organometallic molecules, and metal organic-framework (MOF) systems. The mean absolute errors of GNB are 0.37 kcal/mol for the dispersion and mixed groups of the S66 × 8 benchmark set, 0.35 kcal/mol for CO₂ adsorption on MOF materials, and 4.53 kcal/mol for the XTMC43 benchmark. GNB outperforms existing FF and in many cases has accuracy comparable to that of QM methods such as PBE-D3. GNB can potentially replace the nonbonded part of existing FFs in a wide range of applications.