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Abstract Nature preprograms sophisticated processes in operating molecular machines at the nanoscale, amplifying the molecular motion across multiple length‐scales, and controlling movements in living organisms. Supramolecular soft robotics serve as a new alternative to hard robotics, are able to transform and amplify collective motions of the supramolecularly assembled molecular machines in attaining macroscopic motions, upon photoirradiation. By taking advantage of oriented supramolecular macroscopic soft scaffold, here the first rapid macroscopic movements of supramolecular robotic materials driven by visible light are presented. Head‐tail amphiphilic structure is designed with the phenylazothiazole motif as the photoswitching core. Unidirectionally aligned nanostructures of the amphiphilic phenylazothiazoles are controlled by non‐invasive blue light irradiation and bends toward the light source, demonstrating a fast macroscopic actuation of supramolecular robotic systems (up to 17° s −1 ) in aqueous media. Through meticulous X‐ray diffraction and electron microscopy analyzes, macroscopic actuation mechanism is illustrated in a tight relation to molecular geometric transformations upon photoisomerization. By elucidating the key macroscopic actuation parameters, this paves the way for the next generation design of supramolecular soft robotic systems with enhanced biomimetic actuating functions.
Chau et al. (Wed,) studied this question.