Dielectric properties of nanoconfined water from ab initio thermopotentiostat molecular dynamics

TL;DR

This paper introduces a method to incorporate a thermopotentiostat into ab initio molecular dynamics, enabling first-principles calculation of dielectric properties of water confined at interfaces under constant electrode potential.

Contribution

The paper presents a novel integration of thermopotentiostat technique into AIMD, allowing accurate simulation of interfacial water dielectric response at fixed electrode potential.

Findings

Computed polarization bound charge of interfacial water

Determined dielectric response from first principles

Validated the thermopotentiostat approach for AIMD simulations

Abstract

We discuss how to include our recently proposed thermopotentiostat technique [Phys. Rev. Lett. 126, 136803 (2021)] into any existing ab initio molecular dynamics (AIMD) package. Using thermopotentiostat AIMD simulations in the canonical NVT{\Phi} ensemble at constant electrode potential, we compute the polarization bound charge and dielectric response of interfacial water from first principles.