Chiral Organic Synapses Based on Self‐Assembled Charge‐Transfer Co‐Crystal Helix/TIPS‐Pentacene Heterojunctions

ABSTRACT Chiral neuromorphic devices, representing an advanced synchronous integration of neuromorphic engineering and chiral optoelectronics, offer a new pathway for intelligent computing and high‐dimensional sensing technologies. In this study, a charge‐transfer co‐crystal helical structure based on pyrene and 1,2,4,5‐tetracyanobenzene (TCNB) was prepared via a simple solution process. This structure exhibits chiral emission by virtue of chiral supramolecular assembly, owing to the strong solvent‐solute interactions. To enhance the charge storage performance, a heterojunction with phase‐separated characteristics was constructed by one‐step drop‐casting TIPS‐pentacene and pyrene–TCNB solutions. The heterojunction effectively modulates the interfacial charge trapping and separation processes, thereby enhancing the chiroptical sensitivity. Under optical pulse stimulation, the device simulated multiple synaptic functions, including paired‐pulse facilitation (PPF), pulse‐duration‐dependent and intensity‐dependent plasticity, and biomimetic learning behaviors. This work provides a feasible technological pathway of chiral artificial synapse construct toward photonic neuromorphic computing system developing.