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.