Cooperative Supramolecular Polymerization of Cyanovinylenes for Circularly Polarized Light Photodetection

ABSTRACT Integrating chiral organic molecules as photoactive layers is a promising approach to simplifying device architectures and miniaturizing photodetectors; however, simultaneously achieving low cost and high circularly polarized light (CPL) detection performance remains challenging. Here, we present a cooperative supramolecular polymerization strategy that transforms simple point‐chiral building blocks into long‐range‐ordered chiral supramolecular polymers for CPL‐sensitive organic field‐effect transistor (OFET) photodetectors. Cyanovinylene‐based chromophores were end‐functionalized with commercially available point‐chiral amide groups, enabling spontaneous assembly into chiral supramolecular polymers under appropriate solvent conditions. This point‐chirality‐based molecular design enables facile synthesis and purification, substantially lowering material costs. Cooperative intermolecular hydrogen bonding and π – π stacking drive the formation of long‐range‐ordered helical architectures, effectively transferring and amplifying molecular chirality to the supramolecular level. The resulting mesoscopic assemblies exhibit strong excitonic coupling between adjacent chromophores, leading to a markedly enhanced anisotropic absorption factor ( g _abs ≈ 10 ⁻² ). When employed as photoactive layers in organic field‐effect transistor (OFET) photodetectors, the resulting devices exhibit CPL detection at 532 nm, achieving anisotropic responsivity factors ( g _res ) of 0.22–0.28. This work establishes a low‐cost and effective supramolecular strategy for realizing OFET‐based photodetectors with high CPL detection performance.