The complex-shell interaction energies and the corresponding BSSE are shown in Table . The percentage of E BSSE is computed with respect to the CP values. Our computations reveal that the most expensive TZV2P complex-shell interaction energy contains about 5% of BSSE. The commonly employed DZVP basis set in AIMD simulations 9 yield larger BSSE (about 10%). This could potentially translate into a tighter and thus more structured solvation shell. In Table we show the partial atomic charges of [Fe(bpy) 3 ] 2+ in its HS and LS states obtained from B3LYP-D3(BJ) calculations in vacuum and the CPCM implicit model for water. The total charge of each ligand is also computed to gauge the effect of the solvent on how the charges are distributed. While, in the LS state, polarization from the solvent has negligible effect on the PACs of the complex, the charges were distributed differently in the HS state: When CPCM is used, the PAC of Fe 2+ becomes more negative by ∼0.3e, while the charge of each ligand becomes more positive by ∼0.1e. We then compare the two sets of charges in computing the HS-LS difference of the total interaction energy in the [Fe(bpy 18,19,20). As depicted in Figure , the HS-LS OPLS/TIP4PEW interaction energy differences using PACs obtained from calculations in the gas phase and CPCM solvent model are very similar, although the summed chargedifferences on the ligands and the metal atom differ between the vacuum-and CPCM-derived partial charges. Therefore, the discrepancies between the DFT model and the MM model cannot simply be due to the pairwise additive Coulomb model being fed inaccurate partial charges.