Transferable Water Potentials Using Equivariant Neural Networks

Abstract: Machine learning interatomic potentials (MLIPs) are an emerging modeling technique that promises to provide electronic structure theory accuracy for a fraction of its cost, however, the transferability of MLIPs is a largely unknown factor. Recently, it has been proposed (J. Chem. Phys., 2023, 158, 084111) that MLIPs trained on solely liquid water data cannot describe vapor-liquid equilibrium while recovering the many-body decomposition analysis of gas-phase water clusters, as MLIPs do not directly learn the physically correct interactions of water molecules, limiting transferability. In this work, we show that MLIPs based on an equivariant neural network architecture trained on only 3,200 bulk liquid water structures reproduces liquid-phase water properties (e.g., density within 0.003 g/cm3 between 230 and 365 K), vapor-liquid equilibrium properties up to 550 K, the many-body decomposition analysis of gas-phase water cluster up to six-body interactions, and the relative energy and the vibrational density of states of ice phases. This study highlights that state-of-the-art MLIPs have the potential to develop transferable models for arbitrary phases of water that remain stable in nanosecond-long simulations.