Using machine learning to go beyond potential energy surface benchmarking for chemical reactivity.

Abstract

We train an equivariant machine learning (ML) model to predict energies and forces for hydrogen combustion under conditions of finite temperature and pressure. This challenging case for reactive chemistry illustrates that ML potential energy surfaces are difficult to make complete, due to overreliance on chemical intuition of what data are important for training. Instead, a 'negative design' data acquisition strategy using metadynamics as part of an active learning workflow helps to create a ML model that avoids unforeseen high-energy or unphysical energy configurations. This strategy more rapidly converges the potential energy surfaces such that it is now more efficient to make calls to the external ab initio source when query-by-committee models disagree to further molecular dynamics in time without need for ML retraining. With the hybrid ML-physics model we realize two orders of magnitude reduction in cost, allowing for prediction of the free-energy change in the transition-state mechanism for several hydrogen combustion reaction channels.