Efficient Training of ANN Potentials by Including Atomic Forces via Taylor Expansion and Application to Water and a Transition-Metal Oxide

Abstract

Artificial neural network (ANN) potentials enable the efficient large-scale atomistic modeling of complex materials with near first-principles accuracy. For molecular dynamics simulations, accurate energies and interatomic forces are a prerequisite, but training ANN potentials simultaneously on energies and forces from electronic structure calculations is computationally demanding. Here, we introduce an efficient alternative method for the training of ANN potentials on energy and force information based on an extrapolation of the total energy via a Taylor expansion. By translating the force information to approximate energies, the quadratic scaling with the number of atoms exhibited by conventional force-training methods can be avoided, which enables the training on reference data sets containing complex atomic structures. We demonstrate for different materials systems, clusters of water molecules, bulk liquid water, and a lithium transition-metal oxide, that the proposed force-training approach provides substantial improvements over schemes that train on energies only. Including force information for training reduces the size of the reference data sets required for ANN potential construction, increases the transferability of the potential, and generally improves the force prediction accuracy. For a set of water clusters, the Taylor-expansion approach achieves around 50% of the force error improvement compared to the explicit training on all force components, at a much smaller computational cost. The alternative force training approach thus simplifies the construction of general ANN potentials for the prediction of accurate energies and interatomic forces for diverse types of materials, as demonstrated here for water and a transition-metal oxide.