Abstract
Simulation techniques based on accurate and efficient repre-sentations of potential energy surfaces are urgently needed for the understanding of complex systems such as solid-liquid interfaces. Here we present a machine learning framework that enables the efficient development and validation of models for complex aqueous systems.
Instead of trying to deliver a glob-ally optimal machine learning potential, we propose to develop models applicable to specific thermodynamic state points in a simple and user-friendly process. After an initial ab initio simu-lation, a machine learning potential is constructed with minimum human effort through a data-driven active learning protocol.
Such models can afterward be applied in exhaustive simulations to provide reliable answers for the scientific question at hand or to systematically explore the thermal performance of ab initio methods. We showcase this methodology on a diverse set of aqueous systems comprising bulk water with different ions in solution, water on a titanium dioxide surface, and water con -fined in nanotubes and between molybdenum disulfide sheets.
Highlighting the accuracy of our approach with respect to the underlying ab initio reference, the resulting models are evalu-ated in detail with an automated validation protocol that includes structural and dynamical properties and the precision of the force prediction of the models. Finally, we demonstrate the capa-bilities of our approach for the description of water on the rutile titanium dioxide (110) surface to analyze the structure and mobility of water on this surface.
Such machine learning models provide a straightforward and uncomplicated but accu-rate extension of simulation time and length scales for complex systems.