A “short blanket” dilemma for a state-of-the-art neural network potential for water: Reproducing experimental properties or the physics of the underlying many-body interactions?

Abstract

Deep neural network (DNN) potentials have recently gained popularity in computer simulations of a wide range of molecular systems, from liquids to materials. In this study, we explore the possibility of combining the computational efficiency of the DeePMD framework and the demonstrated accuracy of the MB-pol data-driven, many-body potential to train a DNN potential for large-scale simulations of water across its phase diagram. We find that the DNN potential is able to reliably reproduce the MB-pol results for liquid water, but provides a less accurate description of the vapor–liquid equilibrium properties. This shortcoming is traced back to the inability of the DNN potential to correctly represent many-body interactions. An attempt to explicitly include information about many-body effects results in a new DNN potential that exhibits the opposite performance, being able to correctly reproduce the MB-pol vapor–liquid equilibrium properties, but losing accuracy in the description of the liquid properties. These results suggest that DeePMD-based DNN potentials are not able to correctly “learn” and, consequently, represent many-body interactions, which implies that DNN potentials may have limited ability to predict the properties for state points that are not explicitly included in the training process. The computational efficiency of the DeePMD framework can still be exploited to train DNN potentials on data-driven many-body potentials, which can thus enable large-scale, “chemically accurate” simulations of various molecular systems, with the caveat that the target state points must have been adequately sampled by the reference data-driven many-body potential in order to guarantee a faithful representation of the associated properties.