High-Dimensional Neural Network Potentials for Accurate Prediction of Equation of State: A Case Study of Methane

Machine learning-based interatomic potentials, such as those provided by neural networks, are increasingly important in molecular dynamics simulations. In the present work, we consider the applicability and robustness of machine learning molecular dynamics to predict the equation of state properties of methane by using high-dimensional neural network potentials (HDNNPs). We investigate two different strategies for generating training data: one strategy based upon bulk representations using periodic cells and another strategy based upon clusters of molecules. We assess the accuracy of the trained potentials by predicting the equilibrium mass density for a wide range of thermodynamic conditions to characterize the liquid phase, supercritical fluid, and gas phase, as well as the liquid–vapor coexistence curve. Our results show an excellent agreement with reference phase diagrams, with an average error below ∼2% for all studied phases. Moreover, we confirm the applicability of models trained on cluster data sets for producing accurate and reliable results.