Unprecedented Ultraviolet Circularly Polarized Light‐Dependent Anomalous Photovoltaics in Chiral Hybrid Perovskites

Circularly Polarized Light (CPL)-dependent anomalous photovoltaic effect (APVE), characterized by light helicity-manipulated steady photocurrent and above-bandgap photovoltage, has demonstrated significant potential in the fields of photoelectronic and photovoltaics. However, exploiting CPL-dependent APVE in chiral hybrid perovskites, a promising family with intrinsic chiroptical activity and non-centrosymmetric structure, remains challenging. Here, leveraging the flexible structural design of chiral alternating cations intercalation-type perovskites, CPL-dependent APV, for the first time, is achieved in chiral perovskites. Specifically, by introducing lone pair electrons into the organic layers to greatly amplify the polarization, [(R)-PPA](MOPA)PbBr₄ (2-R) (PPA = 1-phenylpropylammonium, MOPA = 3-methoxypropylammonium) exhibit intrinsic APVE with an above-bandgap photovoltage of 6.50 V (E_g = 3.01 eV) under ultraviolet (UV) light illumination. Strikingly, profiting from the natural chiral optical activity of chiral perovskites, unprecedented UV CPL-dependent APV is realized in 2-R, driving the high distinguishability between right-hand and left-hand CPLs with a large anisotropy factor (g_Iph) of 0.33. This study pioneers the realization of CPL-dependent APV within chiral perovskite, promising significant advancements in optoelectronic device technologies.