Repurposing Existing Molecular Machines through Accurate Regulation of Cooperative Motions

To understand how different external stimuli affect the cooperative motions in a molecular machine consisting of multiple components, we have investigated at the atomic level the effects of pH, solvent, and ionic strength on the mechanism underlying the ring-through-ring movement in a saturated [3]rotaxane. Our results indicate that different external stimuli regulate the stable states, the shuttling rate, and the mechanism that governs the ring-through-ring motion by controlling the cooperative movement of the components and triggering a gamut of responses, thereby opening to a vast number of potential applications, such as quaternary logical calculations. The present work cogently demonstrates that with existing nanomachines possessing a simple topology, but using different external stimuli—an approach coined multidimensional regulation—challenging tasks requiring precise control of the molecular motions at play can be achieved, and our methodology is particularly germane for de novo design of intelligent molecular machines.

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