Highly Efficient Molecular-to-Lattice Chirality Transfer in Benzene-Based Dion–Jacobson Perovskites for Circularly Polarized Light Detection

Chiral organic–inorganic hybrid perovskites are emerging as promising materials for direct detection of circularly polarized light (CPL), yet their performance has remained limited by inefficient chirality transfer and weak interlayer coupling inherent in conventional Ruddlesden–Popper (RP) architectures. In this work, we report benzene-based chiral Dion–Jacobson perovskites based on chiral 1,4-bis(1-aminoethyl)benzene (BDJ)-derived diammonium spacers, which enable highly efficient molecular-to-lattice chirality transfer. Single-crystal X-ray diffraction reveals asymmetric yet deeply penetrating hydrogen-bonding networks, accompanied by pronounced octahedral distortion and strong asymmetry in the Pb–I–Pb angles within the inorganic framework. Consistent with these distinct structural characteristics, BDJ perovskite thin films exhibit exceptionally large circular dichroism with absorption dissymmetry factors (gCD) reaching 0.014. Relative to conventional methylbenzylamine (MBA)-based RP analogues, the BDJ system shows enhanced chiroptical activity as well as a more uniform surface Pb chemical environment. Device-level studies further demonstrate rapid, bias-free CPL-responsive photodiodes exhibiting submillisecond response times and gIph values of 0.12, together with scalable photodetector arrays showing uniform handedness-selective photoresponse and CPL-dependent spatial imaging. These findings highlight chiral BDJ-based perovskites as an effective material platform for circular polarization-sensitive optoelectronics and provide design guidelines for high-performance chiral hybrid perovskites.