Ellipsometric and Raman spectroscopic study of nanocrystalline silicon thin films prepared by a rf magnetron sputtering technique

The structure of nanocrystalline silicon thin films (nc-Si:H) deposited by rf magnetron sputtering of a high-purity crystalline silicon target using argon (30%) and hydrogen (70%) gas mixture, under different pressures (P = 2, 3 and 4 Pa) and different substrate temperature (T(s) = 100, 150 and 200 degrees C), has been studied with spectroscopic ellipsometry (SE; 1.5-5 eV) complemented with Raman spectroscopy measurements. The ellipsometry data were carefully analyzed using the Bruggeman effective medium approximation and the Tauc-Lorentz model. The results of this investigation clearly show that the samples deposited at 2 Pa present a completely amorphous structure whatever the substrate temperature, while those deposited at 3 and 4 Pa exhibit a nanocrystalline structure. These results suggest the existence of a threshold pressure around 3 Pa for which crystallization occurs. The samples are well crystallized with a crystalline volume fraction ranging from about 60 to 90%, and exhibit a mixture of small and large crystallite sizes. The deposition temperature has practically no effect on the size of the crystallites and on the average crystalline volume fractions. These results are in good agreement with the Raman spectroscopy data, and suggest the formation of Si crystallites in the gas phase. The analysis of the ellipsometric spectra also shows that the bulk layer is initiated from an amorphous interface (a-Si:H) present in the first steps of the growth, and is followed by a less crystallized subsurface layer.