[CpFe(CO)(2)](2) (1 : Cp = eta(5)-C5H5) and its permethylated analog [Cp(*)Fe(CO)(2)](2) (1(*) : Cp(*) = eta(5)-C(5)Me(5)) were examined using Raman and resonance Raman spectroscopy. Raman bands associated with high-energy C-O stretches and low-energy Fe-Fe and Fe-(mu-CO) are detected at a variety of excitation wavelengths. The assignments of the C-O stretches and the calculation of carbonyl force constants are presented. The resonance behavior of the C-O stretching modes in 1 and 1(*) is correlated to their lower energy electronic absorption bands, and these results provide an indication of the molecular orbitals involved in the electronic transitions. The spectra show evidence for the formation of the CO-loss photoproducts Cp(2)Fe(2)(mu-CO)(3) (2) and Cp(2)(*)Fe(2)(mu-CO)(3) (2(*)) 2 and 2(*) exhibit rich resonance Raman spectra, including a number of overtones and combination bands of the low-energy vibrational modes. Such spectra suggest a strong coupling between the Fe-Fe stretching and Fe-(mu-CO) breathing modes.