Au Nanocluster Assisted Microstructural Reconstruction for Buried Interface Healing for Enhanced Perovskite Solar Cell Performance

Abstract The heterogeneity of perovskite film crystallization along the vertical direction leads to voids and traps at the buried interfaces, hampering both efficiency and stability of perovskite solar cells. Here, bovine serum albumin‐functionalized Au nanoclusters (ABSA), combined with heavy gravity, high surface charge density, and strong interactions with the electron transport layer, are designed to reconstruct the buried interfaces for not only high‐quality crystallization, but also improved carrier transfer. The ABSA macromolecules with amine function groups and larger surface charge density interact with the perovskite to improve the crystallinity, and gradually migrate towards the buried interface, healing the defective voids, hence suppressing surface recombination velocity from 3075 to 452 cm s −1 . The healed buried interface and the higher surface potential of ABSA‐modified TiO 2 lead to improved carrier extraction at the interface. The resulting solar cell attains a power conversion efficiency of 25.0% with negligible hysteresis and remarkable stability, maintaining 92.9% of their initial efficiency after 3200 h of exposure to the ambient atmosphere, they also exhibit better continuous irradiation stability compared to control devices. These findings provide a new metal‐protein complex to eliminate the deleterious voids and defects at the buried interface for improved photovoltaic performance and stability.