The Raman-active modes of solid films of MxC60 (x-0, 6; M=K, Rb, Cs) and K3C60 have been studied experimentally. The mode-activity is dominated by intraball interactions, and the effect of the M + ions on the C60 spectrum is observed to be almost insensitive to the radius or mass of the alkali metal. Tangential modes of solid C60 are observed to soften in M660 by -60 cm−1, which can be attributed to a charge-transfer-induced elongation of the intraball bond lengths, similar to that observed in graphite intercalation compounds. Conversely, the radial modes are found to upshift slightly, indicating that a competing mechanism counteracts the effect of the bond elongation. For K3C60, six Raman lines have been observed in which the lowest frequency mode exhibits a Breit-Wigner-Fano lineshape, indicating a coupling between the lowest frequency Hq-derived intramolecular modes of C60 and a broad Raman-active continuum with the same symmetry lying lower in frequency.