Abstract

This study investigates the growth process of Ge on Si(100) during atomic-layer epitaxy (ALE) utilizing digermane. The surface ordering, morphology, and stoichiometry of the digermane saturated Si(100) surface at temperatures between 300 and 900 K, as well as the grown films are examined both by scanning tunneling microscopy (STM) and high-resolution core-level photoemission spectroscopy employing synchrotron radiation. An exposure of more than 15 L (1 L=${10}^{\ensuremath{-}6}$ T s) of digermane on the Si(100)-$(2\ifmmode\times\else\texttimes\fi{}1)$ surface at room-temperature results in a saturated and disordered surface. When the digermane saturated surface is heated to 725 K for 60 s, diluted Ge dimer chains are created and surrounded by SiH species. Further annealing to 810 K completely desorbs hydrogen from the surface, leaving large two-dimensional islands covering $\ensuremath{\sim}41%$ of its area. The surface recovers its smooth $2\ifmmode\times\else\texttimes\fi{}1$ structure, but is interspersed with poorly ordered short dimer vacancy lines at 900 K with no observable contrast on the atomic terraces, indicating displacive adsorption of Ge on the terraces. Significant differences of the surface diffusion phenomena between the gas-phase and solid-phase molecular-beam epitaxy (MBE) are observed. Multilayer Si deposition is performed by ALE, i.e., cyclic digermane adsorption at near room temperature, followed by thermal annealing at 900 K. STM images reveal the formation of $2\ifmmode\times\else\texttimes\fi{}n$ structures and increasing roughening of the surface as the growth cycle increases, similar to what occurs during MBE. Issues related to the atomic origins of surface core-level shifts and the chemical composition of the surface layer resulting from the formation of mixed Ge-Si or Ge-Ge during the submonolayer adsorption of Ge on Si(100) are also discussed.

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