Constructing spike-like energy band alignment at the heterointerface in highly efficient perovskite solar cells

The interface between the absorber and transport layers is shown to be critical for highly efficient perovskite solar cells (PSCs). The undesirable physical and chemical properties of interfacial layers often cause unfavorable band alignment and interfacial states that lead to high charge-carrier recombination and eventually result in lower device performance. Herein, we demonstrate a simple and effective strategy to improve the performance of PSCs by constructing a conduction band offset (CBO) with a small spike, through the inductive effect induced by an organic small molecule. As a result, the modified devices show an enhancement in all photovoltaic performance characteristics with a power conversion efficiency (PCE) increase of 10.6% and retaining more than 94% of its initial PCE after 1800 h of exposure to N₂. Importantly, we find that a moderate spike-like CBO at the interface between the perovskite film and hole transport layer facilitates rapid charge-carrier injection in devices and reduces charge recombination at the interface, thereby increasing the open-circuit voltage and fill factor. Furthermore, a large spike barrier at the interface increases device resistance, leading to a reduced fill factor. Our present work provides valuable information for understanding the influence of a spike-like CBO on charge-carrier dynamics to further improve the performance and stability of PSCs.