Ab Initio Thermopotentiostat for Electric Field-Driven Dynamics at the Electrochemical Interfaces

The electrochemical interface plays a crucial role in various energy conversion and storage technologies, as well as in material stability and performance. Controlling the behavior of this interface under dynamic conditions, such as in the presence of external electric fields with ab initio simulations, remains a significant challenge, especially within the periodic density functional theory framework. In this work, we present the development of a thermopotentiostat integrated into an ab initio molecular dynamics (AIMD) framework to design computational electrodes and apply an external electric field to a water-semiconductor interface, specifically for a near-surface point defect in diamond. The system is constructed to maintain charge neutrality while facilitating controlled charge transfer between electrodes, allowing the desired electric field to study its effects on the charge transfer behavior of water to diamond defects. Our results demonstrate that the computational electrodes can generate and sustain electric fields within a temperature-controlled environment. This innovative computational framework provides a new pathway for investigating the influence of electric fields on electrochemical interfaces and offers significant insights for future energy technologies.