J-Aggregates are a class of organic molecules that possess several interesting characteristics that make them attractive for a range of organic-based optoelectronic devices. We present experimental and computer-simulation studies of the Raman-active vibrational modes in the J-aggregate-forming dye 5,6-dichloro-2-[[5,6-dichloro-1-ethyl-3-(4-sulfobutyl)benzimidazol-2-ylidene]propenyl]-1-ethyl-3-(4-sulfobutyl)benzimidazolium hydroxide, sodium salt, inner salt. The molecular monomer and dimer are analyzed computationally and the Raman mode energies extracted. There is a good agreement between the energies of the theoretical and experimental Raman modes. Experimentally, an enhancement is seen in the intensity of two low frequency modes upon aggregation of the dye. This is attributed to aggregation-enhanced Raman scattering. An enhancement is also observed in certain modes of the calculated spectra upon changing from a monomer to dimeric arrangement. A link is suggested between the Raman-active vibrational modes of the molecule, and a time-dependent electronic coupling present over several molecules.