High‐Efficiency Perovskite Solar Cells with Improved Interfacial Charge Extraction by Bridging Molecules

Abstract The interface between the perovskite layer and electron transporting layer is a critical determinate for the performance and stability of perovskite solar cells (PSCs). The heterogeneity of the interface critically affects the carrier dynamics at the buried interface. To address this, a bridging molecule, (2‐aminoethyl)phosphonic acid (AEP), is introduced for the modification of SnO₂/perovskite buried interface in n–i–p structure PSCs. The phosphonic acid group strongly bonds to the SnO₂ surface, effectively suppressing the surface carrier traps and leakage current, and uniforming the surface potential. Meanwhile, the amino group influences the growth of perovskite film, resulting in higher crystallinity, phase purity, and fewer defects. Furthermore, the bridging molecules facilitate the charge extraction at the interface, as indicated by the femtosecond transient reflection (fs‐TR) spectroscopy, leading to champion power conversion efficiency (PCE) of 26.40% (certified 25.98%) for PSCs. Additionally, the strengthened interface enables improved operational durability of ≈1400 h for the unencapsulated PSCs under ISOS‐L‐1I protocol.