To obtain a converged calculated spectrum of CV in methanol, three independent 24 ps MD simulations were performed without the presence of a counterion. The computed absorption spectra based on these individual trajectories produce very similar lineshapes (Fig. ), indicating that slow collective solute-solvent motions are sufficiently sampled even by a small number of trajectories. The average spectrum obtained from these three trajectories correlates well with the experimental data (Fig. ), with the exception of a slight underestimation of the second peak intensity and the overall width of the spectrum. Analysis performed in SI Sec. 5 suggests that the discrepancy in peak heights can be partially ascribed to DFT functional choice, whereas the overall lack in broadening is likely due to neglecting dynamic polarization effects in the spectral density due to representing the solvent environment as fixed classical point charges, as shown by some of our previous work. The results show that the explicit inclusion of the chloride ion in the calculation is not critical for modeling the absorption lineshape of CV in methanol. The splitting between the S 1 and S 2 peaks in the calculated absorption spectrum with and without the counterion is 0.137 eV and 0.141 eV, respectively, compared to the the experimental value of 0.126 eV. The shape of the spectral line indicates that the degeneracy of the HOMO and HOMO-1 orbitals is broken by explicit interactions between CV and its polar solvent environment.