Regulating Charge Transport Dynamics at the Buried Interface and Bulk of Perovskites by Tailored‐phase 2D Crystal Seed Layer

Targeting the trap‐assisted non‐radiative recombination losses and photochemical degradation occurring at the interface and bulk of perovskite, especially the overlooked buried bottom interface, a strategy of tailored‐phase two‐dimensional (TP‐2D) crystal seed layer has been developed to improve the charge transport dynamics at the buried interface and bulk of perovskite films. Using this approach, TP‐2D layer constructed by TP‐2D crystal seeds at the buried interface can induce the formation of homogeneous interface electric field, which effectively suppress the accumulation of charge carriers at the buried interface. Additionally, the presence of TP‐2D crystal seed has a positive effect on the crystallization process of the upper perovskite film, leading to optimized crystal quality and thus promoted charge transport inside bulk perovskites. Ultimately, the best performing PSCs based on TP‐2D layer deliver a power conversion efficiency of 24.58%. The devices exhibit an improved photostability with 88.4% of their initial PCEs being retained after aging under continuous 0.8‐sun illumination for 2000 h in air. Our findings reveal how to regulate the charge transport dynamics of perovskite bulk and interface by introducing homogeneous components.