Machine learning transferable atomic forces for large systems from underconverged molecular fragments

Abstract

Molecular fragments of metal–organic frameworks can be used to construct high-dimensional neural network potentials. Here we provide a recipe of how the smallest possible fragments can be chosen that still provide a HDNNP transferable to the bulk crystal.

Machine learning potentials (MLP) enable atomistic simulations with first-principles accuracy at a small fraction of the costs of electronic structure calculations. Most modern MLPs rely on constructing the potential energy, or a major part of it, as a sum of atomic energies, which are given as a function of the local chemical environments up to a cutoff radius. Since analytic forces are readily available, nowadays it is common practice to make use of both, reference energies and forces, for training these MLPs. This can be computationally demanding since often large systems are required to obtain structurally converged reference forces experienced by atoms in realistic condensed phase environments. In this work we show how density-functional theory calculations of molecular fragments, which are too small to provide such structurally converged forces, can be used to learn forces exhibiting excellent transferability to extended systems. The general procedure and the accuracy of the method are illustrated for metal–organic frameworks using second-generation high-dimensional neural network potentials.