Multi-​scale simulation of electrode interfaces

Abstract

The computational modeling of chem. reactions at electrode interfaces presents extraordinary challenges from the perspective of electronic structure theory. Target applications include electrolyte redn. in formation of the solid-electrolyte interphase (SEI) and the nucleation and growth of metal dendrites. These problems combine large system sizes with subtle interactions, multiple dynamical timescales, and electronically non-adiabatic eects. The development of new methods to perform reliable, on-the-fly electronic structure calcns. at a computational cost that makes feasible the simulation of long-timescale dynamics in large systems remains a central theor. challenge. We describe recent progress towards the development of accurate, scalable treatments for describing battery interfaces. In particular, we will focus on the recent coarse-graining strategies to enable the direct simulation of dendrite formation in lithium metal batteries [1], and we will describe the d. functional theory embedding methods [2, 3] that allow for the accurate description of electrolyte decompn. at metal electrodes.