Great Amplification of Circular Polarization Sensitivity via Heterostructure Engineering of a Chiral Two-Dimensional Hybrid Perovskite Crystal with a Three-Dimensional MAPbI(3) Crystal

[Image: see text] Chiral hybrid perovskites have brought an unprecedented opportunity for circularly polarized light (CPL) detection. However, the circular polarization sensitivity of such a detector remains extremely low because of the high exciton recombination rate in those single-phase hybrid perovskites. Here, a heterostructure construction strategy is proposed to reduce the electron–hole recombination rate in a chiral hybrid perovskite and achieve CPL detectors with greatly amplified circular polarization sensitivity. A heterostructure crystal, namely, [(R)-MPA](2)MAPb(2)I(7)/MAPbI(3) ((R)-MPA = (R)-methylphenethylamine, MA = methylammonium), has been successfully created by integrating a chiral two-dimensional (2D) perovskite with its three-dimensional counterpart via solution-processed heteroepitaxy. Strikingly, the sharp interface of the as-grown heterostructure crystal facilitates the formation of a built-in electric field, enabling the combined concepts of charge transfer and chirality transfer, which effectively reduces the recombination probability for photogenerated carriers while retaining chiroptical activity of chiral 2D perovskite. Thereby, the resultant CPL detector exhibits significantly amplified circular polarization sensitivity at zero bias with an impressive anisotropy factor up to 0.67, which is about six times higher than that of the single-phase [(R)-MPA](2)MAPb(2)I(7) (0.1). As a proof-of-concept, the strategy we presented here enables a novel path to modulate circular polarization sensitivity and will be helpful to design chiral hybrid perovskites for advanced chiroptical devices.