Interfacial Energy Level Alignment and Defect Passivation by Using a Multifunctional Molecular for Efficient and Stable Perovskite Solar Cells

Abstract Tin oxide (SnO₂) is currently the dominating electron transport material (ETL) used in state‐of‐the‐art perovskite solar cells (PSCs). However, there are amounts of defects distributed at the interface between ETL and perovskite to deteriorate PSC performance. Herein, a molecule bridging layer is built by incorporating 2,5‐dichloroterephthalic acid (DCTPA) into the interface between the SnO₂ and perovskites to achieve better energy level alignment and superior interfacial contact. The multifunctional molecular bridging layer not only can passivate the trap states of Sn dangling bonds and oxygen vacancies resulting in improved conductivity and the electron extraction of SnO₂ but also can regulate the perovskite crystal growth and reduce defect‐assisted nonradiative recombination due to its strong interaction with undercoordinated lead ions. As a result, the DCTPA‐modified PSCs achieve champion power conversion efficiencies (PCEs) of 23.25% and 20.23% for an active area of 0.15 cm² device and 17.52 cm² mini‐module, respectively. Moreover, the perovskite films and PSCs based on DCTPA modification show excellent long‐term stability. The unencapsulated target device can maintain over 90% of the initial PCE after 1000 h under ambient air. This strategy guides design methods of molecule bridging layer at the interface between SnO₂ and perovskite to improve the performance of PSCs .