We report an atomic force microscopic (AFM) examination of the photo-induced surface reconstruction of C 60 single crystals. The (111) and the (001) faces of C 60 single crystals were illuminated with photons with energies below the band gap (generation of Frenkel-type excitons) or above the band gap. In the case of sub-band-gap illumination, reconstructed surfaces formed on the crystals. The reconstruction was represented by fringes running in the [112] and [010] directions on the (111) and (001) surfaces, respectively. As a result of supra-band-gap illumination, however, there appeared only cracks, without any fringes, which were oriented in directions characteristic of each face. The results suggest that the photo-induced surface reconstruction of C 60 single crystals is induced via the recombination of Frenkeltype excitons.Since the discovery of C 60 [1], there have been numerous investigations on its structural and optical properties in the solid state [2]. Molecules of C 60 condense at room temperature into a face-centered cubic (fcc) structure held by rather weak intermolecular van der Waals forces [3]. A great number of studies of the surface morphology of epitaxial fullerene films on various types of substrate [4,5] have been conducted with atomic force microscopy (AFM) and/or scanning tunneling microscopy (STM). We recently also carried out AFM studies of the morphology and surface dislocations of fullerene single crystals and epitaxial films [6][7][8][9][10][11]. The reconstructed (0001) face of C 70 single crystals exhibited a long-range periodic array of partial dislocation fringes [8]. In a related fashion, AFM images of the reconstructed surface of C 60 epitaxial films on KBr(001) substrates showed many fringes in the equivalent [110] directions on the fcc(111) plane [11]. In the latter case, molecular-resolution images revealed that the reconstructed surface is contracted by ca. 3% in the [112] direction. Both of these observations suggest a stacking-faultdomain model involving periodic transitions between fcc and hexagonal-closed packed (hcp) structures in the surface layer.Solid C 60 is a molecular semiconductor with a band gap of 2.3 eV [12], and weak optical absorption in the range of 1.6 to 2.2 eV, which corresponds to Frenkel-type excitons [12,13]. Previous to the present work, several reports have appeared concerning photo-transformations of solid C 60 by optical illumination. First, the irradiation of oxygen-free C 60 films with an Ar-ion laser at 514.5 nm (2.41 eV) and 488.0 nm (2.54 eV) was focused to initiate the irreversible polymerization of C 60 [14][15][16]. Second, in the presence of oxygen, C 60 undergoes oxidation upon uv light irradiation [17,18]. Both the photo-induced polymerization and the photoinduced oxidation processes are initiated by supra-band-gap illumination. In this paper, we report an AFM investigation of photo-induced structural transformations of C 60 singlecrystal surfaces using both sub-band-gap and supra-band-gap illumination.