A Methodology for Simulating Solid-Liquid Interfaces Using Many-Body Perturbation Theory

The solid-liquid interface is crucial in interfacial physics and applications such as batteries and catalysis. However, its complexity—arising from the interactions between solid materials and liquids—presents significant challenges for understanding these phenomena. To address this, we developed a methodology based on many-body perturbation theory. This approach utilizes the GW approximation for the electronic structure of solids and employs an implicit model based on the generalized Poisson equation for liquids. Our method accurately predicts the band edge positions of materials in solution and reveals structure-property relationships in porous materials. We further enhanced this methodology by integrating the Bethe-Salpeter equation (BSE) to analyze the optical spectra of solvated materials. This integration successfully reproduces their solvatochromic behavior and provides strategies for controlling their optical properties when submerged. Additionally, we advanced our model to include explicit representations of the liquid phase through molecular dynamics simulations, enabling us to investigate the interfacial structure of liquid molecules. By applying a voltage to the simulation cell containing the electrolyte, we were able to simulate photoelectrochemical interfaces effectively. Finally, I will discuss potential extensions of this method for spectroscopy simulations and introduce a machine learning model designed to accelerate these simulations.