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The deposition of amorphous and epitaxial silicon thin films on H-terminated Si(100) has been studied in real time by the simultaneous application of spectroscopic ellipsometry, attenuated total reflection infrared spectroscopy, and optical second-harmonic generation. The morphology development of the films could be monitored nonintrusively in terms of critical point resonances and H bonding resolving the abruptness of the film-substrate interface and providing a clear distinction between direct heterointerface formation, nanometer-level epitaxial growth, and epitaxial breakdown.