Grain Boundaries Contribute to the Performance of Perovskite Solar Cells by Promoting Charge Separations

Historically seen as a limitation, grain boundaries (GBs) within polycrystalline metal halide perovskite (MHP) films are thought to impede charge transport, adversely impacting the efficiency of perovskite solar cells (PSCs). In this study, we employ home-built confocal photoluminescence microscopy, combined with photocurrent detection modules, to directly visualize the carrier dynamics in the MHP film of PSCs under real operating conditions. Our findings suggest that GBs in high-efficiency PSCs function as carrier transport channels, where a notable enhancement in photocurrent is observed. Femtosecond transient absorption and Kelvin probe force microscopy measurements further validate the existence of a built-in electric field in the vicinity of GBs, offering additional driving force for charge separation and establishing channels for swift carrier transport along the GBs, thereby expediting subsequent charge collection processes. This study elucidates the pivotal role of GBs in operational PSCs and provides valuable insights for the fabrication of high-efficiency PSCs.