Chiral-Polar Photovoltage-Driven Efficient Self-Powered Circularly Polarized Light Detection in Three-Dimensional Hybrid Perovskites

The chiral-polar photovoltaic effect (CPPE), widely present in chiral hybrid perovskites, has brought an unprecedented opportunity for self-powered circularly polarized light (CPL) detection. However, on account of spatial limitations of the crystal structure, currently reported CPPE primarily focuses on low-dimensional hybrid perovskites, which have a low CPL photoresponse restricted by lower carrier transport efficiency compared to three-dimensional perovskites. For the first time, we reported chiral-polar photovoltage-driven efficient self-powered CPL detection in three-dimensional chiral-polar perovskites, MHyPbBr₃ (MHy = Methylhydrazinium). Coupled with significant spontaneous polarization (17.1 μC cm^-2) and superior semiconductor properties, MHyPbBr₃ exhibits a large mobility-lifetime product (1.9 × 10^-2 cm² V^-1) and stable bulk photovoltage (3.9 V). Furthermore, the devices indicate significant chiral-polar photovoltage for self-powered CPL detection with a robust angle anisotropy factor of 0.39. More importantly, benefiting from excellent carrier transport performance, high responsivity and detectivity values of up to 39.2 mA W^-1 and 5.8 × 10¹² Jones, respectively, are presented at zero bias, which fall around the highest values of hybrid perovskites. This work will contribute to the research of novel chiral-polar three-dimensional hybrid perovskite semiconductors and promote their application in efficient self-powered CPL detection.