The combination of 2D and 3D perovskites to passivate surfaces or interfaces with a high concentration of defects shows great promise for improving the efficiency of perovskite solar cells (PSCs). Constructing high-quality perovskite film systems by precisely modulating 2D perovskites with good morphologies and growth sites on 3D perovskite films remains a formidable challenge due to the complexity of spacer-engineered surface reactions. In this study, phase-pure 2D (HA)2(MA)n-1PbnI3n+1 perovskites with a controlled number of layers (n) are separated on a large scale and exploited as interface rivets to optimize 3D perovskite films, resulting in tunable film structural defects and grain boundaries. The optimized PSCs system benefits from a reduction in non-radiative recombination, resulting in improved optical performance, higher mobility, and lower trap density. The corresponding device achieves a champion power conversion efficiency (PCE) of more than 25%, especially for voltage (VOC) and fill factor (FF). The quality and uniformity of the perovskite films are further confirmed using large-area devices with an active area of 14 cm2, which exhibits a PCE of more than 21.24%. The high-quality thin-film system based on the 2D perovskites presented herein provides a new perspective for improving the efficiency and stability of PSCs.
Keywords: (HA)2(MA)n−1PbnI3n+1 perovskites; 2D/3D perovskite solar cells; 2D/3D perovskites; grain boundaries; high‐quality thin‐film systems.
© 2023 Wiley‐VCH GmbH.