Cooperative Supramolecular Polymerization of Cyanovinylenes for Circularly Polarized Light Photodetection.

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