Raman spectra of the spin-crossover complex Fe(phen)(2)(NCS)(2) in the solid state have been recorded at 785 nm as a function of temperature to investigate the contribution of intramolecular vibrations to the entropy change, Delta S, associated with spin crossover. The modes of major interest for estimating the contribution lie in the range 100-500 cm(-1), where the largest qualitative changes with temperature in the Raman spectra were observed. Analysis of these data, with the working assumption of an average frequency in this range as representative of the 15 distortion modes of an idealised FeN6 octahedron, leads to the conclusion that the intramolecular vibrations represent a primary contribution to the total Delta S.