First, while all QM/MM MD calculations are initialized with Cl -in a contact ion pair configuration taken from CV in vacuum, all trajectories equilibrate to the same configuration distinct from the optimized vacuum configuration, that remains stable over 10s of ps, suggesting that the contact-ion pairing is indeed highly stable. We have tested other initial configurations for Cl -, such as the ideal position chosen by AMBER to minimize the electrostatic potential, yielding similar final spectra (see SI Sec. 2). While the position of the counterion in the real solution might be combination of contact ion pairings and configurations with the ions further separated, the strong-electrostatic interactions in nonpolar solvents and the long-timescale stability of the contact-ion pairing in our simulation means we likely sufficiently sample the configurations that dominate the experimental lineshape. Second, we have carried out calculations where Cl -is included in the QM region for both the QM/MM dynamics and the calculation of vertical excitation energies (see SI Sec. 5), with only minor influence on the resulting spectra, confirming that a FF treatment of Cl - is not a dominant factor in the discrepancy with experimental lineshapes. Finally, we note that for the strongly symmetry-broken configuration caused by direct contact ion pairing, the S 1 state of CV has significantly less charge-transfer (CT) character than the S 2 state. This causes functionals with different treatment of long-range exchange to predict a range of S 1 -S 2 splittings for the same CV-Cl -configurations (see SI Sec. 5), with the CAM-B3LYP functional resulting in a much closer agreement with experiment for a short QM/MM trajectory of CV in toluene (Fig. ). However, the CAM-B3LYP functional does not yield the correct description of CV in Methanol, significantly overestimating the intensity of the second spectral peak (Fig. ), suggesting that due to the different strengths of environmental symmetry breaking, standard DFT functionals do not describe CV in both condensed phase environments equally well. We conclude that the dominant factor causing the discrepancy between computed spectra of CV in toluene and experiment is likely errors in description of the CT character of the symmetry-broken S 2 state in the (TD)DFT calculations of vertical excitation energies.