Manipulating perovskite structural asymmetry for high-performing self-powered full-stokes polarimetry

Chen et al., Sci. Adv. 11, eads6123 (2025) 28 February 2025 S c i e n c e A d va n c e s | R e s e a r c h A r t i c l e 1 of 10 M AT E R I A L S S C I E N C E Manipulating perovskite structural asymmetry for high-­performing self-­powered full-­stokes polarimetry Quanlin Chen1,2†, Mingwei Ge3†, Cong Geng1, Jia Zhang1, Linyue Gao1, Zhuanzhuan Huang4, Saike Wang1, Yanxing Feng1, Xinxin Yue4, Saif M. H. Qaid5, Xuewen Fu4, Mei Wang6*, Yuanzhi Jiang1*, Mingjian Yuan1* Developing direct full-­stokes imaging polarimetry is essential for various applications but remains challenging. Perovskites have superior optoelectronic properties and structural diversity, making them ideal candidates for high-­performing direct full-­stokes polarimetry. However, perovskite suffers low chiroptical activity due to ineffi- cient chiral transfer, which greatly limits its circular-­polarization-­vector discrimination. These issues urgently re- quire remedy. Here, we demonstrate that perovskites’ chiroptical activity is highly related to their structural chiral-­distortion extent. We propose using halide mixing to construct asymmetric chiral transfer to heighten its structural chiral-­distortion extent. Accordingly, we report a 16-­fold increment in the optical chiroptical activity. Further ab initio calculations verify that the enhancement is due to the strengthened magnetic transition dipole in mixed-­halide structures. We herein report a self-­powered, direct full-­Stokes polarimetry with a high detectivity up to 1.2 × 1012 Jones and low detection errors (ΔS1–3 ≤ 5.0%). We further showcase their application in full-­stokes imaging polarimetry with the lowest detection errors yet. INTRODUCTION To gain more comprehensive information about the objectives, it is highly essential to realize high-­performing full-­stokes imaging po- larimetry that can capture both light intensity and polarization states (1–4). Currently, state-­of-­the-­art full-­stokes polarization detection technology relies on polarimetry coupled with integrated metasur- face or grating components (5–7). However, integrating optical parts introduces serious optical losses and manufacturing complexities, greatly restricting their application in next-­generation miniaturized portable devices. Developing semiconductors with intrinsic polarization sensitiv- ity offers an alternative approach to realize full-­stokes imaging po- larimetry with high-­sensitivity and minimized footprint (8, 9). This requires the semiconductor’s structure to exhibit both anisotropic and chiral characteristics, which demands precise control over their lattice geometric configuration (10). However, it remains challeng- ing to implant both anisotropic and chiral features in conventional semiconductors due to their limited structural diversity. Hybrid organic-­inorganic perovskites have attracted widespread attention due to their exceptional semiconducting properties. Their structural diversity further serves as a versatile platform for function-­ oriented structure design (11, 12). For instance, ligand intercalation– induced structural anisotropy has been realized in low-­dimensional perovskites, enabling efficient linearly polarized light (LPL) detec- tion (13). In addition, chiral perovskites can be constructed via asymmetric hydrogen bonds (H bonds)–induced structural distor- tion, facilitating circularly polarized light (CPL) detection (14, 15). Accordingly, perovskites with both anisotropic and chiral characteris- tics are ideal candidates for efficient direct full-­Stokes detection. How- ever, efficiently incorporating both asymmetric features in perovskites remains unexplored. In particular, the chiral transfer and amplifica- tion in perovskites remain extremely inefficient, resulting in poor over- all chiroptical activity (16, 17). Here, we report a bismuth-­halide–based zero-­dimensional perovskite, (R/S-­MBA)4Bi2Br10, which has both anisotropic and chiral crystal- lograph