Programmable Engineering of Sunlight-Fueled, Full-Wavelength-Tunable, and Chirality-Invertible Helical Superstructures

Dynamic control of motion at the molecular level is a core issue in promoting the bottom-up programmable modulation of sophisticated self-organized superstructures. Self-assembled artificial nanoarchitectures through subtle noncovalent interactions are indispensable for diverse applications. Here, the active solar renewable energy is used to harness cholesteric liquid crystal (CLC) superstructure devices via delicate control of the dynamic equilibrium between the concentrations of molecular motor molecules with opposite handedness. Thus, the spectral position and handedness of a photonic superstructure can be tuned continuously, bidirectionally, and reversibly within the entire working spectrum (from near-ultraviolet to the thermal infrared region, over 2 mu m). With these unique horizons, three advanced photoresponsive chiroptical devices, namely, a mirrorless laser, an optical vortex generator, and an encrypted contactless photorewritable board, are successfully demonstrated. The sunlight-fueled chirality inversion prompts facile switching of functionalities, such as free-space optical communication, stereoscopic display technology, and spin-to-orbital angular momentum conversion. Motor-based chiroptic devices with dynamic and versatility controllability, fast response, ecofriendly characteristics, stability, and high efficiency have potential to replace the traditional elements with static functions. The inexhaustible natural power provides a promising means for outdoor-use optics and nanophotonics.

Automated summary

This study focuses on the dynamic control of motion at the molecular level to promote programmable modulation of sophisticated self-organized superstructures. By utilizing solar renewable energy, the spectral position and handedness of a photonic superstructure can be continuously and reversibly tuned. Advanced photoresponsive chiroptical devices have potential to replace traditional elements with their ecofriendly characteristics, fast response, stability, and high efficiency.