Robust Spin-Dependent Anisotropy of Circularly Polarized Light Detection from Achiral Layered Hybrid Perovskite Ferroelectric Crystals

Circularly polarized light (CPL) detection has sparked overwhelming research interest for its widespread chiroptoelectronic and spintronic applications. Ferroelectric materials, especially emerging layered hybrid perovskite ferroelectrics, exhibiting striking bulk photovoltaic effect (BPVE) present significant possibilities for CPL detection by a distinctive working concept. Herein, for the first time, we demonstrate the realization of robust angular anisotropy of CPL detection in a new layered hybrid perovskite ferroelectric crystal (CPA)₂FAPb₂Br₇ (1, CPA is chloropropylammonium, FA is formamidinium), which crystallized in an optically active achiral polar point group. Benefiting from the notable spontaneous polarization (5.1 μC/cm²) and excellent semiconducting characteristics, single crystals of 1 exhibit remarkable BPVE under light illumination, with a high current on/off switching ratio (ca. 10³). More intriguingly, driven by the angular carrier drift originating from spin-dependent BPVE in optically active ferroelectrics, 1 displays highly sensitive self-powered CPL detection performance, showing a robust angular anisotropy factor up to 0.98, which is far more than those achieved by material intrinsic chirality. This work provides an unprecedented approach for realizing highly sensitive CPL detection, which sheds light on the further design of optically active ferroelectrics for chiral photonic applications.