Double-layer step formation on Si(100) substrates is a crucial prerequisite for antiphase-domain free III-V compound semiconductor heteroepitaxy. Due to its unequaled relevance in microelectronics, the (100) oriented surface of silicon is by far the most studied semiconductor surface. However, Si(100) preparation in hydrogen process gas ambient, which is commonly employed for Si and III-V device preparation, is completely different from preparation in ultra-high vacuum due to strong interaction

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... between H 2 and the Si surface, leading to a kinetically driven different step formation. Here, we observe chemical layer-by-layer removal of surface atoms from the terraces at the Si(100) surface during annealing in hydrogen ambient. Mutually perpendicularly oriented dimers on subsequently removed monolayers induce oscillations in the in situ reflection anisotropy spectroscopy (RAS) signal. Scanning tunneling microscopy measurements support a model, where surface