The dark side of the forces: assessing non-conservative force models for atomistic machine learning

Abstract

The use of machine learning to estimate the energy of a group of atoms, and the forces that drive them to more stable configurations, has revolutionized the fields of computational chemistry and materials discovery. In this domain, rigorous enforcement of symmetry and conservation laws has traditionally been considered essential. For this reason, interatomic forces are usually computed as the derivatives of the potential energy, ensuring energy conservation. Several recent works have questioned this physically constrained approach, suggesting that directly predicting the forces yields a better trade-off between accuracy and computational efficiency, and that energy conservation can be learned during training. This work investigates the applicability of such non-conservative models in microscopic simulations. We identify and demonstrate several fundamental issues, from ill-defined convergence of geometry optimization to instability in various types of molecular dynamics. Given the difficulty in monitoring and correcting the lack of energy conservation, direct forces should be used with great care. We show that the best approach to exploit the acceleration they afford is to use them in conjunction with conservative forces. A model can be pre-trained efficiently on direct forces, then fine-tuned using backpropagation. At evaluation time, both force types can be used together to avoid unphysical effects while still benefitting almost entirely from the computational efficiency of direct forces.