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The surface reaction kinetics of Si thermal oxidation was investigated by a real-time monitoring method of Auger electron spectroscopy combined with reflection high-energy electron diffraction. From the time evolution of O KLL Auger electron intensity measured simultaneously with that of RHEED intensity, thermal oxidation on the Si(001) surface under an O2 pressure of 2×10-7 Torr was divided into three temperature regions: (1) Langmuir-type adsorption at T < 630oC, (2) two-dimensional (2D) SiO2 island growth at 630oC < T < 800oC, and (3) etching (active oxidation) at 800oC < T. In the temperature region of 2D SiO2 island growth, an oscillatory behavior of RHEED half-order spot intensity of (1/2, 0) and (0, 1/2) was observed, indicating layer-by-layer etching of the surface between SiO2 islands. The RHEED intensity oscillation was accompanied with an appearance of bulk diffraction spots in RHEED patterns, suggesting a development of protrusions under the SiO2 islands, however no bulk diffraction spots were observed in other two regions. On the basis of the correlation between SiO2 coverage and RHEED intensity of specular, half-order and bulk diffraction spots, the time evolution of surface morphology is discussed for Langmuir-type adsorption and 2D SiO2 island growth.

Real-time Monitoring of Si Thermal Oxidation by Auger Electron Spectroscopy Combined with Reflection High-Energy Electron Diffraction.