Abstract

AbstractControl over geometric curvature and chirality of assemblies in pure aqueous media is key to the design of responsive materials and molecular machines. Here we show how aggregate geometric curvature and chirality of motor amphiphiles could be switched from bicontinuous calabashes to nanoribbons or from vesicles to nanoribbons by modulating rotor orientation direction with dual light/heat stimuli to influence spontaneous curvature in assemblies. The photoisomerization and thermal helix inversion processes of molecular motors have been studied at the molecular level, and the transformation of supramolecular assemblies has been investigated at the microscopic level. The morphological evolution of the calabash‐shaped assembly can be kinetically captured, suggesting that the bicontinuous calabash‐shaped structures are different from the bowl‐shaped aggregates based on solvent‐driven assembly upon the addition of non‐solvent or solvent. The investigation of dual optical/thermal control of rotor orientation can provide a new strategy for tuning the geometric curvature and chirality of nanoassemblies at the nanoscale, arriving ultimately the clusteroluminescence through‐space electronic communication at responsive supramolecular nanosystems.

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