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We investigated transition layers at the interface of the thin SiO2 film successively etched back by diluted HF, using infrared reflection-absorption spectroscopy. The etching rate of the oxide film reveals that there is a Si-rich transition layer within 0.6 nm of the interface. However, frequency shift in the longitudinal optical phonon due to Si-O-Si asymmetric stretching toward lower wave numbers takes place less than 1.5 nm from the interface. We propose a model in which the transition layer is assumed to be Si-rich suboxide layers caused by the compositional roughness of the SiO2/Si interface. Through estimating the phonon frequencies which depend on the composition of the suboxide structure in this model, we found that the phonon frequency apparently starts to shift at around 1.5 nm from the interface, even if there are suboxide-rich layers within 0.6 nm, which can be caused by 1–2 monolayers of roughness.

We investigated bonding configurations of nitrogen atoms in silicon oxynitride films, resulting in a 960 cm−1 absorption peak, which is a higher frequency than that for Si3N4 (840 cm−1). The 960 cm−1 peak was observed in the films for which an N 1s x-ray photoemission peak was observed with a binding energy of about 398.6 eV, which has been reported as a binding energy associated with the ≡Si–N–Si≡ structure. However, the 960 cm−1 peak was absent in the films for which the N 1s peak was observed at about 397.8 eV, being close to the binding energy associated with the Si3≡N structure. We conclude that the absorption peak at 960 cm−1 arises from the ≡Si–N–Si≡ structure of doubly bonded N atoms with two Si atoms, not affected by any oxygen atoms.

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