For both compounds, the QM calculations with openCOSMO-RS and QM-GNNIS show a good correlation between their predicted populations and the experimental J tot values. In contrast, QM calculations with SMD show no correlation for 2-methoxy-ethanol and a weaker one for compound 1,2-dimethoxyethane. This finding is especially interesting as the SMD implicit-solvent model showed the best correlations for the molecular balances (Fig. ), indicating that this good performance may likely be only because of the strong correlation with the dielectric permittivity of the solvent in case of the molecular balances. As alluded to in the Introduction (Fig. ), the relatively low population of the trans-conformer in water may be attributed to the formation of a pseudo-seven-membered ring via a hydrogen-bond network of a water molecule with 2-methoxy-ethanol . The lower trans-conformer population in water predicted by QM-GNNIS and openCOSMO-RS with respect to other polar solvents (i.e., methanol and DMSO) demonstrates that the approach can capture more complex solute-solvent interactions.