Elucidating Solvatochromic Shifts in Two-Dimensional Photocatalysts by Solving the Bethe-Salpeter Equation Coupled with Implicit Solvation Method.

Many studies have focused on tailoring the photophysical properties of two-dimensional (2D) materials for photocatalytic (PC) or photoelectrochemical (PEC) applications. To understand the optical properties of 2D materials in solution, we established a computational method that combined the Bethe-Salpeter equation (BSE) calculations with our GW-GPE method, allowing for GW/BSE-level calculations with implicit solvation described using the generalized Poisson equation (GPE). We applied this method to MoS 2 , phosphorene (PP), and g -C 3 N 4 and found that when the solvent dielectric increased, it reduced the exciton binding energy and quasiparticle bandgap, resulting in almost no solvatochromic shift in the excitonic peaks of MoS 2 and PP, which is consistent with previous experiments. However, our calculations predicted that the solvent dielectric had a significant impact on the excitonic properties of g -C 3 N 4 , exhibiting a large solvatochromic shift. We expect that our GW/BSE-GPE method will offer insights into the design of 2D materials for PC and PEC applications.