Factors influencing charge transport at perovskite-charge transport layer interfaces: current strategies, challenges, and perspectives based on first-principles studies

Charge transport at the interface between a perovskite absorbing layer and the charge transport layer (CTL) has a major role in determining perovskite solar cell device efficiency and long-term stability. Hence, a detailed operando characterization of the factors influencing charge transport at perovskite/CTL interfaces needs to be discussed. This perspective summarizes recent studies involving charge transport through perovskite and CTL interfaces. An overview is provided of the recent advances in the fundamental understanding of how these interfaces influence device performance. Based on recently reported articles, some of the crucial factors such as energy-level alignment, defects, and non-radiative recombination are identified. The identification is made from an atomistic point of view as these factors have a strong influence on charge transport at perovskite/CTL interfaces. Furthermore, we share our perspective on calculating said factors influencing interfacial charge transport from different approaches using density functional theory (DFT) and beyond.