Space‐Resolved Photoresponse in Quasi‐Two‐Dimensional Ruddlesden–Popper Perovskites

Abstract Quasi‐two‐dimensional (quasi‐2D) organic–inorganic hybrid perovskites have shown excellent ambient stability with decent photovoltaic performance. Further improvement of device level properties requires a comprehensive understanding of the performance‐limiting mechanisms such as phase segregation, ion/electron coupling conduction, and their effects on charge transport at both the micro‐ and macro‐scale. Here, space resolved investigations of Ruddlesden–Popper (RP) phases of the commonquasi‐2D perovskite are probed using two complementary methods, conducting atomic force microscopy (c‐AFM) and Kelvin probe force microscopy (KPFM). Bias‐driven photocurrent mappings obtained by c‐AFM measurements disclose local inhomogeneous conduction and hysteresis currents in quasi‐2D RP perovskites, while relatively uniform conductivity is observed on individual grains. Bias‐driven KPFM reveals that the surface average photovoltage sign is dominated by the band bending at the buried perovskite–substrate interface. The quasi‐2D RP film exhibits substantial variations in the spatial response of the photovoltage across grains and grain boundaries, which is direct evidence of the inherently benign nature of microstructures, and the final device performance. This research elucidates underlying space‐resolved photoresponse mechanisms behind the lower efficiency of quasi‐2D RP perovskites compared with the 3D perovskites, which is necessary for further development of efficient and stable 2D perovskite‐based devices.