Chiral Cyclic Dimeric Pyromellitic Diimides Single‐Crystalline Arrays for Integrated Circularly Polarized Solar‐Blind Ultraviolet Photodetector

ABSTRACT Circularly polarized light (CPL) detection in the solar‐blind ultraviolet (UV range (200–280 nm) holds promise for applications in secure communication, environmental monitoring, and near‐earth communication due to its low background noise and high signal‐to‐noise ratio. However, the balance between the high absorption asymmetry factors ( g _abs ) and efficient electronic transport have restricted organic solar‐blind UV CPL detection. Herein, we present chiral cyclic pyromellitic diimide ((−)‐ and (+)‐2PMDI), exhibiting a maximum absorption peak at 235 nm. Its D ₂ symmetry gives a 180° or 0° angle between the magnetic ( m ) and electric transition ( µ ) dipole moments, contributing to high | g _abs | of 0.01. The self‐assembled single‐crystalline microwire arrays of (+)‐2PMDI with favorable π−π stacking are fabricated by multi‐interface confined assembly strategy as active layers of solar‐blind UV photodetectors, which exhibit excellent stability, a maximum responsivity ( R ) and detectivity ( D ^* ) of 3.73 × 10 ⁻³ A W ⁻¹ and 5.01 × 10 ⁸ Jones. Based on these photodetectors, we further demonstrate the integrated CPL imaging with high resolution of 37 × 37 pixels, and devices show a photocurrent asymmetry factor ( g _ph ) of 0.39. This study provides fundamental new insight into chiral organic integrated optoelectronics for CPL solar‐blind UV photodetection.