• TDDFT/TDA calculations in the subspace of standard DMET embedding orbitals yield slightly more accurate excitation energies (and higher r 2 values) than TDA/TIP3P and TDA/EFP models, confirming the importance of entangling the occupied orbitals on the chromophore and solvent molecules. However, for a further better description of the virtual space, one needs to utilize a generalized density matrix that is augmented by contributions from full-system virtual orbitals to acquire the DMET bath orbitals, thus highlighting the key role of entanglement between the virtual orbitals on the chromophore and solvent molecules. The entanglement between chromophore and solvent virtual orbitals plays a particularly important role for pHBDI -.