Surface reaction of CH4 on the Si(1 0 0) epitaxial surface was investigated in the low-temperature region of 500-750°C at 50-1600 Pa for 7-240 min using an ultraclean vertical-type hot-wall LPCVD system. In the case of the CH4 exposure at ≥650°C, the reacted C atom diffused into Si and a SiC layer was formed. At ≤550°C, CH4 reacted with Si only at the surface without apparent diffusion, and the 4-fold periodic structure toward the [0 0 1] azimuth was formed on the surface. At 600°C, with increasing exposure time, the 4-fold periodic structure was initially formed and then disappeared and the diffraction spots of SiC appeared, which indicates substantial diffusion of the reacted C atom into Si. Furthermore, at ≤600°C, the reacted C atom concentration at the outermost surface was normalized with the product of the CH4 pressure and the exposure time, and was expressed by the Langmuir-type rate equation.
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