High‐Performance Circularly Polarized Light Photodetector via Temperature and High‐Energy Photons Modulation in 1D Chiral Perovskite Single Crystals

Abstract The chiroptical properties of perovskites offer a direct means for optical detection and discrimination of polarization information. inefficient chirality transfer from organic chiral spacers to the inorganic framework leads to generally low anisotropy factors ( g res ) in circularly polarized light (CPL) detection. In contrast, 1D chiral perovskites exhibit superior chirality, thereby generating significantly enhanced CPL responses. Centimeter‐scaled and block‐shaped 1D chiral perovskite single crystals (SCs) (R)‐/(S)‐AMEPYPb 2 Br 6 (AMEPY = 2‐aminoethyl‐1‐methylpyrrolidine) are grown, with intrinsic chirality for circularly polarized light (CPL) discrimination. Theoretical analysis reveals that charge transport routes (intrachain/interchain) and efficiency are dynamically modulated by thermal lattice distortion and photoexcited states. By optimizing free‐carrier capture probability and trap‐state density, the resulting CPL photodetector demonstrates an anisotropy factor of 1.05 for (S)‐AMEPYPb 2 Br 6 and −1.12 for (R)‐AMEPYPb 2 Br 6 along the intrachain direction , representing a two‐fold improvement over reported perovskite materials. Equally importantly, A responsivity of 1.97 A W −1 and detectivity of 3.8 × 10 12 Jones are also achieved, along with excellent bias and UV‐light stability, comparable to commercial diodes.