Photoprogrammable Mesogenic Soft Helical Architectures: A Promising Avenue toward Future Chiro‐Optics

Abstract Mesogenic soft materials, having single or multiple mesogen moieties per molecule, commonly exhibit typical self‐organization characteristics, which promotes the formation of elegant helical superstructures or supramolecular assemblies in chiral environments. Such helical superstructures play key roles in the propagation of circularly polarized light and display optical properties with prominent handedness, that is, chiro‐optical properties. The leveraging of light to program the chiro‐optical properties of such mesogenic helical soft materials by homogeneously dispersing photosensitive chiral material into an achiral soft system or covalently connecting photochromic moieties to the molecules has attracted considerable attention in terms of materials, properties, and potential applications and has been a thriving topic in both fundamental science and application engineering. State‐of‐the‐art technologies are described in terms of the material design, synthesis, properties, and modulation of photoprogrammable chiro‐optical mesogenic soft helical architectures. Additionally, the scientific issues and technical problems that hinder further development of these materials for use in various fields are outlined and discussed. Such photoprogrammable mesogenic soft helical materials are competitive candidates for use in stimulus‐controllable chiro‐optical devices with high optical efficiency, stable optical properties, and easy miniaturization, facilitating the future integration and systemization of chiro‐optical chips in photonics, photochemistry, biomedical engineering, chemical engineering, and beyond.