Additionally, we examined the influence of different inner-sphere sizes (8-24 Å) on the pseudo-translational and pseudo-rotational contributions within a single snapshot (see Fig. in the Supporting Information). The results show that further increasing the size of the inner sphere has a minor effect on the pseudo-translational and pseudo-rotational contributions of acetone in water. This observation is anticipated, as only the solvent molecules in close proximity to the core region interact strongly with it.