Publication date: 6th November 2020
Electrochemical technologies are considered crucial to future sustainable energy scenarios. However, the complexity of these systems has hindered the first-principles understanding and design of materials for such energy conversions. I'll describe our approaches to understand electrochemical reactions based on a grand-canonical---or constant-voltage---approach to atomistic simulations, and how these calculations can be directly linked to experimental observations. I will cover the methodology we have developed, which we refer to as the "solvated jellium" approach, which enables electronically grand-canonical calculations to run at comparable cost to canonical calculations. A key ramification of processes at constant potential is that the number of electrons involved in a reaction is not known a priori, and is not in general an integer quantity. Examples will be provided on how we use these approaches to inform and guide experiments.