A practical computational protocol for photocatalytic reactions beyond ground-state approximations

Abstract

Theoretical studies of heterogeneous photocatalysts typically discuss the band level alignment obtained by ground-state DFT, which does not capture the physics of light-driven processes. Here, we present a new computational protocol in which excited states are explicitly considered in the Gibbs free energy diagrams. This is applied to prototypical H₂O oxidation and O₂ reduction reactions on a single-atom Co-embedded g-C₃N₄ cocatalyst.