Enabling multilevel optical communication via photo-triggered macroscopic phase evolution in cholesteric liquid...

The advancement of next-generation optical computing and secure communication necessitates the development of molecular triggers capable of driving definitive, cross-scale transitions within ordered soft matter. Herein, we demonstrate a function-oriented design of a quaternary optical logic platform enabled by the first class of chiral bipolar A-D-A structured donor-acceptor Stenhouse adducts (Bi-DASAs). By engineering the molecular framework to maximize electronic perturbations, we achieve a reversible, visible-light-driven isomerization characterized by a significant reconfiguration of the molecular dipole moment and a 221° reorientation. These amplified molecular drivers facilitate the self-assembly of cholesteric (Ch) superstructures, which serve as the physical substrate for multi-state logic gate implementation. Mechanistic investigations reveal that the macroscopic Ch-nematic (N) phase transition is synergistically driven by the light-induced attenuation of molecular chirality and the reconstruction of guest-host dipole-dipole interactions. By digitizing these discrete, power-dependent phase states, we develop a spatial light modulator prototype capable of quaternary digital signaling and high-bandwidth alphanumeric data transmission. Furthermore, we implement an optical comparator logic system for secure authentication, showcasing the practical utility of Bi-DASA-based architectures in high-density information processing and adaptive optoelectronics. Our findings establish a robust modular strategy for programming complex optical logic through molecular-level dipole-switching.