Bridged Carbolong Modulating Interfacial Charge Transfer Enhancement for High‐Performance Inverted Perovskite Solar Cells

Efficient regulation of perovskite/C60 interface is crucial to improving the long‐term stability of the inverted perovskite solar cells (PSCs). However, precise methods for controlling the perovskite/C60 interface have yet to be thoroughly explored. Herein, we develop a carbolong chemical manipulation strategy to improve the interface contact of perovskite/C60 due to versatile functional groups and excellent optoelectronic properties of carbolong metallaaromatics. And constructing an electron‐transfer bridge enhances the interfacial interaction and accelerates interfacial electron transfer. The carbolong manipulation results in optimized energy level alignment, suppressed nonradiative recombination, and improved electronic contact. An impressive efficiency of 25.80% is demonstrated, with open‐circuit voltage and fill factor of 1.19 V and 84.53%, respectively. The unsealed devices retain more than 98% of their original efficiency after 1400 h of maximum power point tracking under illumination and demonstrate remarkable thermal stability, maintaining 93% of their initial efficiency after 2500 h at 85°C in a nitrogen atmosphere. And the encapsulated carbolong‐modified module achieved a high efficiency of 20.72% (active area of 25.25 cm²) with robust operation stability.