CB[5]@CB[10]. Dynamics and Interaction Energy Considerations in a Molecular Gyroscope from MD+EDA Calculations

Supramolecular noncovalent interactions infer flexibility desired to enable functional motion and molecular machinery, favoring the development of complex molecular machines at the nanoscale. Here, we evaluate the dynamical behavior of supramolecular gyroscane-like complexes, given by CB[5]@CB[10] and Cl@CB[5]@CB[10]−. Our results denote that noncoaxial conformations are energetically favored due to reduced Pauli repulsion and enhanced electrostatic interactions, from a combined molecular dynamics (MD) simulations and energy decomposition analysis (EDA), denoted as MD+EDA approach, the intricate gyroscope-like rotational and precessional motions between the inner CB[5] unit and the outer CB[10] cavity are revealed, showing the impact of further incorporation of anions to modulating the supramolecular interaction dynamics. The MD+EDA approach elucidates fluctuating energy contributions during motion, showing that chloride inclusion buffers electrostatic stabilization and facilitates freer molecular motion. These findings advance understanding of noncovalent interactions governing dynamic supramolecular assemblies and provide foundational insights for designing artificial molecular machines with controllable, multifunctional motion.