The CV + and methanol QM/MM AIMD configurations presumably have errors due to the QM/MM interface, which affect the interaction of the chromophore and solvent. The MM treatment of solvent during the QM/MM AIMD may lead to over-polarization of the QM region, and therefore closer chromophore-solvent distances, potentially leading to the weaker vibronic coupling seen in our computed spectral density and high-frequency absorption spectrum. As a test of this hypothesis, we computed the Franck-Condon spectrum of CV + in methanol in both frozen MM solvent and frozen QM solvent environments for one frame from the QM/MM trajectory. We applied an Ohmic implicit solvent broadening parameter to the computed Franck-Condon spectra corresponding to a solvent reorganization energy of λ = 0.001 a.u., see SI. For computation with a full QM solvent shell, we use the same 5 Å QM solvent shell as in our vertical excitation energy calculations described above (≈ 230 QM atoms). The ground state and excited state geometry of the QM chromophore was optimized and normal modes computed in the field of the fixed solvent. These adiabatic Hessian Franck-Condon spectra show that additional vibronic broadening occurs with the QM treatment of the solvent environment, with the computed Franck-Condon spectrum producing a broader vibronic shoulder than in experiment, see Figure . Note that this additional vibronic broadening must come from the change in the position of the chromophore relative to the solvent associated with the QM treatment of the first solvation shell. The static Franck-Condon spectrum with frozen MM solvent highly resembles the dynamic cumulant spectrum from the QM/MM AIMD trajectory with the excitation energies calculated with MM solvent (comparing the solid red lines in panels (a) and (b) of Fig. ), showing that the two spectral simulation methods are consistent within this QM/MM model.