Anchoring Vertical Dipole to Enable Efficient Charge Extraction for High‐Performance Perovskite Solar Cells

Abstract Perovskite solar cells (PSCs) via two‐step sequential method have received great attention in recent years due to their high reproducibility and low processing costs. However, the relatively high trap‐state density and poor charge carrier extraction efficiency pose challenges. Herein, highly efficient and stable PSCs via a two‐step sequential method are fabricated using organic—inorganic (OI) complexes as multifunctional interlayers. In addition to reduce the under‐coordinated Pb2+ ions related trap states by forming interactions with the functional groups, the complexes interlayer tends to form dipole moment which can enhance the built‐in electric field, thus facilitating charge carrier extraction. Consequently, with rational molecular design, the resulting devices with a vertical dipole moment that parallels with the built‐in electric field yield a champion efficiency of 23.55% with negligible hysteresis. More importantly, the hydrophobicity of the (OI) complexes contributes to an excellent ambient stability of the resulting device with 91% of initial efficiency maintained after 3000 h storage.