Crystal Violet (CV) is a triarylmethane dye with compelling optical properties. The low-energy absorption lineshape of CV contains two peaks, the splitting between which depends on the solvent and temperature. 1 Korppi-Tommola and Yip observed that the overlap between absorption bands strongly depends on the solvent polarity, so that in nonpolar solvents there are two distinct peaks, whereas in polar solvents the bands overlap strongly. The nature of the higher energy peak has been debated for decades and remains uncertain. There are two main theories describing this phenomenon: 1) the ground state of CV is inhomogeneous and this causes the appearance of the second peak in absorption lineshape; or 2) solute-solvent interactions induce the D 3 symmetry of CV to break and cause the lifting of the degeneracy of the excited state. For instance, Lewis et al. suggested the idea that in a solvent there is a thermal equilibrium between two isomers of CV 1 one of those is symmetrical helical type (D 3 symmetry) and the other one is distorted helical type (C 2 symmetry). Even though the existence of the particular C 2 isomer was not supported by the experiment, the D 3 isomerization was confirmed by femtosecond pumpprobe measurement. Maruyama et al. suggested that the structural changes between the two ground states cannot be large, so that CV is present as a planar D 3 a) Electronic mail: tim.zuehlsdorff@oregonstate.edu configuration and a pyramidal C 3 configuration. The calculated absorption bands of these isomers in ethanol agreed well with the experiment. Korppi-Tommola and Yip hold a different point of view, suggesting that the degeneracy of the S 1 state is lifted due to solvation in polar solvents and interaction with a counterion in nonpolar ones, the last interaction being stronger, which leads to greater separation between the absorption bands. This theory was supported by McHale et al. using polarized resonance Raman scattering, fluorescence emission data, and semiempirical molecular orbitals (MO) calculations, the latter were also used to indicate the energy barrier for torsional isomerization, which was found to exceed k B T , thus is was shown that rotation of the phenyl groups is unlikely. However, Lovell et al. later stated, based on the polarization and analysis of the previous studies, that the two theories are not mutually exclusive, and that the ground state of CV exists as an equilibrium of two isomers, one of which has a non-degenerate S 1 state. Additionally, it was shown that the absorption lineshape depends on the solvatochromic parameters of the solvent, again arguing against the inhomogeneity of the ground state. The most recent studies either do not support both theories, or suggest that the center of the absorption band of CV corresponds to the excitation of the symmetric molecule, and the edges correspond to the S 1 and S 2 transitions of the symmetry-broken molecules according to QM calculations and time-resolved polarized spectroscopy data. Thus, the dominant factor in the appearance of a shoulder in absorption spectrum of CV remains unclear, and can be ascribed to either the existence of two isomers of the ground state, torsional disorder of the molecule, environmental interactions, or a combination of these factors.