Resonance Raman spectra and cross sections of a "push-pull" chromophore containing a julolidine donor and a thiobarbituric acid acceptor have been measured in dilute solution in five solvents having a wide range of polarities (cyclohexane, 1,4-dioxane, dichloromethane, acetonitrile, and methanol) at excitation wavelengths spanning the strong visible charge-transfer absorption band. The absolute Raman excitation, profiles and absorption spectra are simulated using time-dependent wave packet propagation techniques to determine the excited-state geometry changes along the similar to 30 Raman-active vibrations as well as the solvent reorganization energies. Several vibrational modes undergo significant (5-15 cm(-1)) frequency changes as the solvent is varied, signaling solvent polarity effects on the ground-state electronic structure. The excited-state geometry changes are solvent dependent for some vibrational modes but not for others. The total vibrational reorganization energy decreases, and the solvent reorganization energy increases with increasing solvent polarity in all solvents except the one protic solvent, methanol, which is anomalous in both respects. Tentative assignments are made for the ground-state vibrational modes by comparison of the Raman frequencies and infrared frequencies and intensities with those calculated using density functional theory, as well as by comparison with model compounds. The results are discussed within the context of the two-state valence-bond model for the electronic properties of conjugated push-pull chromophores.