Pseudo‐Arch Bridge‐Inspired Stress Modulation at Buried Interface for Stable High‐Efficiency Perovskite Solar Cells

/perovskite interface likely in a unique "molecular bridge" configuration. This soft interface yields an extremely low modulus and significantly reduces the interfacial stress energy from 0.554 to 0.178 eV, thereby suppressing defect formation and minimizing phase segregation. Meanwhile, the functional groups in FBI-PyAI passivate defects and induce vertically oriented perovskite crystallization, forming compact films with fewer voids and improved structural uniformity. As a result, the modified devices achieve exceptional thermal stability, which maintains 88% of initial efficiency after 50 thermal cycles (-15 to 65 °C). Moreover, the modified PSC delivers a competitive efficiency of 25.01% and outstanding photostability (95% retention after 800 h illumination under ISOS-L-1 protocol). This work offers mechanistic insight into interfacial stress modulation and underscores its importance for thermally stable PSCs.