Fullerene C-60 thin films were grown by physical vapor deposition (PVD) onto Si (1 0 0) substrates at room temperature in a vacuum chamber kept at 10(-6) Torr. Photopolymerization of C-60 was performed by irradiation with a pulsed Kr-F laser. The films obtained at a fluence of 25 mJ/cm(2) were no longer soluble in toluene, indicating the conversion Of C60 into a different solid phase. IR spectra of the irradiated films exhibit several new intense modes indicating the lowering of fullerene molecule symmetry. At the same time, the characteristic modes of pristine C-60 had reduced intensities or disappeared, indicating the contribution of sp(3)-bonding. Raman spectra of the modified C-60 films showed the lowering of C-60 symmetry as well, along with the increasing disorder due to sp(3) carbon atoms. The highest applied irradiation of above 30 mJ/cm(2) resulted in the broadening of G and D-bands related to the amorphous carbon phase. The optimal experimental conditions for fullerene photopolymerization for areas larger than 1 cm, reducing the undesirable formation of other carbon phases, were found. (c) 2005 Elsevier B.V. All rights reserved.