Control on dissipative kinetics reveals the entropically-dominated essence of interlocked molecular machines

Abstract

The operation of nanomachines is fundamentally different from that of their macroscopic counterparts. In particular, the role of solvent is critical, yet rarely associated with machine functionality. Here we study a minimal model of one of the most advanced molecular machines, to gain control on its operation by engineering components and the employed solvent. Operation kinetics was modulated over more than four orders of magnitude, and could be fine-tuned. Leveraging solvent properties, it was possible to realize multiple cycles of the molecular machine operation while monitoring it. Our work expands the capabilities of acid-base powered molecular machines, contributing to the development of systems that leverage solvent properties to expand their functionality.