A pH-responsive and Redox-Driven Tristable [2]Rotaxane

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From a broader perspective, this work contributes to the rationalization of multistate mechanically interlocked systems by establishing a robust computational protocol capable of resolving the subtle interplay of noncovalent interactions governing positional equilibria. The combined use of DFT with implicit solvation, together with topological and real-space analyses such as QTAIM and IGMH, provides a transferable framework that can be extended to more complex and functionally integrated rotaxane architectures. In particular, future developments may target the predictive design of higher-order stimuli-responsive systems, including multi-input molecular logic devices and adaptive supramolecular assemblies operating under competitive environmental conditions. Moreover, the explicit inclusion of dynamic effects, counterions, and more realistic solvent representations could further refine the quantitative description of switching mechanisms. Ultimately, approaches of this kind are expected to accelerate the transition from empirical synthesis toward fully design-driven molecular engineering, enabling the development of next-generation molecular machines with programmable behavior and enhanced operational reliability.

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