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In this study, by controlling source temperature, substrate temperature, and growth time, C60 polycrystalline films are prepared by physical vapor deposition. Meanwhile, the surface morphology, films thickness, degree of crystallinity, and optical absorption of the as-grown C60 polycrystalline films are characterized by scanning electron microscopy, X-ray diffraction, and temperature-dependent optical transmission (with incident photon energies from 1.46 ~ 2.07 eV), respectively. Based on the experimental results from C60 polycrystalline films, the variation of averaged grain size (R) versus film thickness (L) can be categorized by three regimes. At the very beginning, R varies with L following the equation: R L0.72. As L approaches 1 ~ 2 μm, R saturates around 1 μm and at this moment the ITO surface is completely covered by C60 polycrystalline grains. In the second regime, as the growth proceeds, R varies with L0.91 until L reaches 10 ~ 20 μm, and then R saturates around 10 μm again. In the third regime, R varies with L1.18. In addition, form the optical transmission spectra of C60 polycrystalline films with L = 5 ~ 20 μm, three pairs of absorption peaks can be resolved as Ea = 1.848 eV, Ea’ = 1.880 eV, Eb = 1.940 eV, Eb’ = 1.968 eV, Ec = 2.016 eV, and Ec’ = 2.045 eV. Furthermore, four absorption peaks of E1 = 1.688 eV, E2 = 1.719 eV, E3 = 1.747 eV, and E4 = 1.777 eV can be recognized in the spectra of thick C60 polycrystalline films with L = 52 ~ 60 μm. These rich variations of absorption peaks can be explained by the Herzberg-Teller coupling (electronic-vibronic interaction) in this organic molecular solid. Then, an energy terms diagram is proposed for the band structure of solid C60 fullerite. This model assumes that the valence band and conduction band in this polycrystalline sample are composed by the Davydov splitting from molecular levels of S0 and S1, respectively. So, the energy bandgap (Eg) is defined and then Eg(T) is performed for this solid C60 fullerite. Finally, from a numerical fit of Eg(T) to O’Donnell-Chen equation, the fitting parameters are obtained for these C60 polycrystalline thick-films, and a comparison of these fitting
parameters to those obtained from C60 single crystals is made.