With reducing diamond grain size to nano-grade, the increase of grain boundaries and non-diamond phase will result in the change of the optical properties of chemical vapor deposition (CVD) diamond films. In this paper, the structure, morphology and optical properties of nanocrystalline diamond (NCD) films, deposited by hot-filament chemical vapor deposition (HFCVD) method under different carbon concentration, are investigated by SEM, Raman scattering spectroscopy, as well as optical transmission spectra and spectroscopic ellipsometry. With increasing the carbon concentration during the film deposition, the diamond grain size is reduced and thus a smooth diamond film can be obtained. According to the data on the absorption coefficient in the wavelength range from 200 to 1100 nm, the optical gap of the NCD films decreases from 4.3 eV to 3.2 eV with increasing the carbon concentration from 2.0% to 3.0%. From the fitting results on the spectroscopic ellipsometric data with a four-layer model in the photon energy range of 0.75–1.5 eV, we can find the diamond film has a lower refractive index (n) and a higher extinction coefficient (k) when the carbon concentration increases.
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