ABSTRACTWe have developed optical models for the characterization of grain size in nanocrystal thin films embedded in SiO2 and fabricated using low pressure chemical vapor deposition of Si from silane on a quartz substrate, followed by thermal oxidation. The as-grown nanocrystals thin film on quartz was composed of a two-dimensional array of Si nanocrystals (Si-NC) showing columnar structure in the z-direction and touching each other in the x-y plane. The nanocrystal size in the z-direction was equal to the Si nanocrystal film thickness, changing by the deposition time, while their x-y size was almost equal in all the samples, with small size dispersion. After high temperature thermal oxidation, a thin silicon oxide film was formed on top of the nanocrystals layer. The aim of this work was to measure the grain size and the nanocrystallinity of the Si nanocrystal thin films, a quantity related to the change of the dielectric function. We used a definition for the nanorcystallinity that is related to the effective medium analysis (EMA) of the material. The optical technique used for the investigations was spectroscopic ellipsometry. To measure the above sample properties the thickness and composition of several layers on a quartz substrate had to be determined by proper modeling of this complex system. We found that the nanocrystallinity (defined as the ratio of nc-Si/(c-Si+nc-Si) decreases systematically with increasing the Si-NC layer thickness. Using this approach we are sensitive to the lifetime broadening of electrons caused by the scattering on the grain boundaries, and not to the shift of the direct interband transition energies due to quantum confinement.