Effect of ligand groups on photoexcited charge carrier dynamics at the perovskite/TiO₂ interface

The work proposed here aims to describe the dynamics of photoexcited charge carriers at the interface between the perovskite and electron transport layer (ETL) in perovskite solar cells (PSCs) and the effect that the interface morphology has on these dynamics. This is done in an effort to further develop the understanding of these materials so that their chemical composition and morphology may be better utilized to improve PSCs by means of increasing the power conversion efficiency (PCE), maximizing the chemical stability of PSCs to lengthen their lifespan, finding the cheapest and easiest materials to synthesize which have beneficial properties in photovoltaics, etc. This is done by using density functional theory to model the interface and open system Redfield theory to describe the charge carrier dynamics. We find that the charge transfer characteristics at the perovskite/ETL interface depend greatly on the choice of ligands adsorbed on the ETL that act as a bridge between the perovskite and ETL. The two ligand choices discussed here go so far as to determine whether the system will undergo a Förster energy transfer or a Dexter energy transfer upon photoexcitation.