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We present a systematic study of the local hydrogen bonding in hydrogenated polymorphous silicon thin films (pm-Si:H), a heterogeneous material deposited on the edge of crystallinity, by means of Fourier transform infrared spectroscopy. A vibrational mode at similar to2030 cm(-1) is reported and attributed to hydrogen atoms bonded in hydrogen-rich regions present at the interface between ordered regions and the amorphous matrix. This assignment is found to be in good agreement with previous spectroscopic ellipsometry and Raman spectroscopy studies. Combined with stress measurements we draw a picture of the nanostructure of pm-Si:H films, namely a two-domain material exhibiting: (i) large fluctuations of H content, (ii) a high mass density and (iii) the coexistence of highly strained crystalline phases with a relaxed amorphous matrix. Unexplained optoelectronic properties and metastability phenomena can also be accounted for by this picture.

Hydrogenated polymorphous silicon (pm-Si:H) is a new material obtained by plasma-enhanced chemical vapour deposition by running the plasma close to powder formation. Preliminary studies have revealed the presence of silicon nanocrystallites embedded in an amorphous matrix but only in a limited range of deposition conditions. In this work we have investigated the structural properties of such films by means of spectroscopic optical measurements. The analysis of transmission spectra in the transparent region has shown that pm-Si:H films have indeed a more ordered structure than state-of-the-art hydrogenated amorphous silicon (a-Si:H) films. This has been observed in the whole range of deposition conditions leading to pm-Si:H films. On a final point the implication of structural properties on the excellent optoelectronic properties previously reported in pm-Si:H films is discussed.