The surface composition is measured during atomic layer epitaxy (ALE) growth of Si on Ge(100) using Si2Cl6 and atomic hydrogen (Hat) at TS=400 °C. During each Si2Cl6 exposure, Si is adsorbed until Cl fully terminates the surface, making the Si deposition step self‐limiting. The terminating Cl layer is removed by Hat exposure. At 400 °C, H2 rapidly desorbs from Ge(100) and Si/Ge alloy surfaces, regenerating the surface dangling bonds for the next Si2Cl6 adsorption cycle. A thin alloy is grown epitaxially on the Ge(100) substrate, which displays a linear increase in Si content and a linear decrease in Ge content, measured over 1–20 Si ALE cycles.

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