Molecular machines operated by light have been recently shown to be able to produce oriented motion at the molecular scale^1,2 as well as do macroscopic work when embedded in supramolecular structures^3,4,5. However, any supramolecular movement irremediably ceases as soon as the concentration of the interconverting molecular motors or switches reaches a photo-stationary state^6,7. To circumvent this limitation, researchers have typically relied on establishing oscillating illumination conditions—either by modulating the source intensity^8,9 or by using bespoke illumination arrangements^10,11,12,13. In contrast, here we report a supramolecular system in which the emergence of oscillating patterns is encoded at the molecular level. Our system comprises chiral liquid crystal structures that revolve continuously when illuminated, under the action of embedded light-driven molecular motors. The rotation at the supramolecular level is sustained by the diffusion of the motors away from a localized illumination area. Above a critical irradiation power, we observe a spontaneous symmetry breaking that dictates the directionality of the supramolecular rotation. The interplay between the twist of the supramolecular structure and the diffusion¹⁴ of the chiral molecular motors creates continuous, regular and unidirectional rotation of the liquid crystal structure under non-equilibrium conditions.

最近显示，由光操作的分子机器能够在分子尺度^1,2产生定向运动，并且嵌入超分子结构^3,4,5时也能进行宏观工作。但是，一旦分子间转换的分子马达或开关的浓度达到光平稳状态^6,7，任何超分子运动都将不可避免地停止。为了避免这种局限性，研究人员通常依靠建立振荡照明条件-通过调制光源强度^8,9或使用定制照明装置^10,11,12,13。相反，这里我们报告了一个超分子系统，其中振荡模式的出现是在分子水平上编码的。我们的系统包括手性液晶结构，该结构在嵌入式光驱动分子马达的作用下被照亮时会不断旋转。超分子水平上的旋转通过电机扩散远离局部照明区域而得以维持。在临界辐射功率以上，我们观察到自发对称断裂，该断裂决定了超分子旋转的方向性。超分子结构的扭曲和手性分子马达的扩散¹⁴之间的相互作用产生了在非平衡条件下液晶结构的连续，规则和单向旋转。