The structures of the studied molecular balances are shown in Fig. and the experimentally determined freeenergy differences between the indicated ketone rotational states using 19 F{ 1 H} NMR measurements were taken from Ref. . The starting structures for the molecular balances were taken from Ref. . There, a representative ensemble based on 5120 KDG conformers was generated using the minimization approach with the classical GNNIS model for each balance in each of the nine solvents. These structures were then optimized using the BP86 functional with the SVP basis set and a D4 correction . Next, their free energies were assessed in the nine different solvents for all implicit-solvent models according to the above description. Note that for QM-GNNIS, some conformers showed imaginary frequencies after the ASE minimization. As these do not represent true minima, these conformers were excluded from further analysis. The free energies of the minimized conformers were then used to calculate the populations of the two rotamers based on the ketone rotation shown in Fig. . In order to focus the analysis on the differences in these free-energy differences, ∆∆G, with respect to different solvents, the means of the experimental and predicted free energies were subtracted from the experimental and predicted free energies, respectively, for each balance. Note that data points, which only represent upper boundaries (i.e., populations lower than the detection limit of the NMR procedure), were not included in the comparison. SciPy (version 1.10.1) was used to calculate the Pearson correlation coefficient (PCC) and the linear least-squares regression between the experimental and predicted ∆∆G.