Light‐Triggered Sustainable Defect‐Passivation for Stable Perovskite Photovoltaics

Abstract The generation of photoinduced defects and freely moving halogen ions is dynamically updated in real time. Accordingly, most reported strategies are static and short‐term, which make their improvements in photostability very limited. Therefore, seeking new passivation strategies to match the dynamic characteristics of defect generation is very urgent. Without newly generated defects, a passivation molecule should exist in the configuration that would not become the initiation sites for defect generation. With newly generated defects, the passivation molecule should transfer into the other configuration that possesses the passivation sites. Herein, a classical photoisomeric molecule, spiropyran, is adopted, whose pre‐ and post‐isomeric forms meet the requirements for two different configurations, to realize the state transition once the photoinduced defects appear during subsequent operation and dynamic capture for continuous renewal of defects. Consequently, spiropyrans work as light‐triggered and self‐healing sustainable passivation sites to realize continuous defect repair. The target devices retain 93% and 99% of their initial power conversion efficiencies after 456 h aging under ultraviolet illumination and 1200 h aging under full‐spectrum illumination, respectively. This work provides a novel concept of sustainable passivation strategy to realize continuous defect‐passivation and film‐healing in perovskite photovoltaics.