Large-scale quantum atomistic electrochemistry simulations

We are developing software tools for atomistic electrochemical simulations under operational conditions. These new computational tools are not only capturing the essential chemistry and physics of devices such as batteries but can also give us the parameters needed for bridging atomistic with larger scale simulations. Our developments are within the ONETEP program [1] which is based on a linear-scaling reformulation of density functional theory (DFT) that allows atomistic simulations of orders of magnitude more atoms than conventional approaches, so that we can construct more realistic models. In this talk I will outline our developments so far which include methods for metallic systems, solvent and electrolyte models [2], and a grand-canonical approach which allows simulations at fixed voltage with respect to a computational reference electrode [3-4]. Finally I will present an application of these methods in recent simulations of the process of lithium metal deposition on anodes, which is a common mechanism for battery degradation [5].