The CCSD-HF, sc-TS and FCO-MBD methods qualitatively agree in predicting charge redistribution due to electronic correlations. FCO-MBD accurately describes density polarization in the intermonomer region, while discrepancies near the nuclei stem from the harmonic potential approximation in MBD, which differs from the full Coulomb potential. The self-consistent sc-TS method agrees more closely with CCSD in the density tails, suggesting the importance of self-consistency, which is the focus of ongoing work on FCO-MBD. The isosurfaces of ∆ρ(r) displayed in Figure witness that ∆ρ pol (r) from FCO-MBD captures the key features of ∆ρ CCSD-HF (r) redistribution also in 3D space. The remaining differences outside monomers can be attributed to the dipole coupling approximation used in the MBD model. In addition, the CCSD-HF difference includes contributions other than dispersion, e.g. the difference in electronic polarization between CCSD and HF. In methane dimer, this difference is small, whereas in relatively more polarizable dimers like pentane this effect may contribute to the difference between CCSD and MBD (Figure ). Ambrosetti et al. further demonstrated that the fully-coupled MBD model can semi-quantitatively reproduce molecular optical excitation spectra. This ensures that the fully-coupled MBD method delivers physically sound description of collective quasi-plasmonic fluctuation modes, interplay of which creates a vdW-induced polarization of electronic density.