We have used an atomic force microscope to analyze the surface of C60thin films, which have been grown epitaxially on a mica surface and illuminated with a 514.5 nm laser light at different temperatures. Two regimes of light-induced polymerization are observed. If the illumination temperatureTpis lower than 320 K, the illuminated surface shows polymer chains typically six molecules long with an intermolecular distance of 9.2±0.1Å . Because of the strain associated with the shorter inter-C60distance in the polymer compared to the bulk, the surface is buckled with a period of∼100 Å and amplitude of ∼5 Å resulting in a characteristic herringbone three-dimensional structure. For films, illuminated above 350 K, the surface shows primarily dimers and trimers with an unusually short inter-C60distance of8.8±0.1Å, this being the shortest interbuckyball distance reported so far. We also find large changes in the adhesive forces on the polymerized films compared to unpolymerized ones, suggesting that the polymer is substantially more hydrophyllic than normal C60.©1997 American Institute of Physics.