Neural network atomistic potentials for global energy minima search in carbon clusters

Abstract

The global energy optimization problem is an acute and important problem in chemistry. It is crucial to know the geometry of the lowest energy isomer (global minimum, GM) of a given compound for the evaluation of its chemical and physical properties. This problem is especially relevant for atomic clusters. Due to the exponential growth of the number of local minima geometries with the increase of the number of atoms in the cluster, it is important to find a computationally efficient and reliable method to navigate the energy landscape and locate a true global minima structure. Newly developed neural network (NN) atomistic potentials offer a numerically efficient and relatively accurate approach for molecular structure optimization. An important question that needs to be answered is “Can NN potentials, trained on a given set, represent the potential energy surface (PES) of a neighboring domain?”. In this work, we tested the applicability of ANI-1ccx and ANI-nr NN atomistic potentials for the global minima optimization of carbon clusters C_n (n = 3–10). We showed that with the introduction of the cluster connectivity restriction and consequent DFT or ab initio calculations, ANI-1ccx and ANI-nr can be considered as robust PES pre-samplers that can capture the GM structure even for large clusters such as C₂₀.