Meng Su, Xudong Wu, JiBin ZHANG, Meng Wang, Jingli Ma, Linyuan Lian, Conghui Dun, Qinglin Zeng, Q. Liu, Yongtao Tian, Xu Chen, Mochen JIA, Ying Liu, Yanbin Han, Zhuangzhuang Ma, Di Wu, Xinjian Li, Zhifeng SHI
ABSTRACT 1D chiral perovskites, exhibiting anisotropic and chiroptical activities, are highly promising candidates for full‐Stokes polarization detection. However, inefficient chirality transfer in these materials results in weak chiroptical responses, seriously limiting their capability for circular polarization discrimination. Here, we develop a facile Sb 3 ⁺ doping strategy to effectively modulate the structural asymmetry of ( R/S ‐3AD)PbBr 3 Cl·H 2 O crystals (3AD = 3‐aminopiperidine dihydrochloride), significantly enhancing the chirality transfer from chiral organic components to inorganic framework owing to the symmetry‐breaking lattice distortions and yielding a 30‐fold increase in chiroptical activity. Furthermore, the doped chiral perovskite crystals exhibit a pronounced Dember effect, enabling self‐driven photodetection. As a result, the Sb 3 ⁺‐doped ( R/S ‐3AD)PbBr 3 Cl·H 2 O crystals achieve a maximum circular polarization sensitivity factor of 0.44 and a linear polarization ratio of 1.43 at zero bias, allowing accurate full‐Stokes polarization detection with a Stokes parameter averaging error below 7%. This study offers a new strategy for boosting the chiroptical responses in chiral perovskites and presents the first demonstration of self‐driven full‐Stokes photodetection via the Dember effect.