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The electronic structure of Si‐doped GaAs layers grown by molecular‐beam epitaxy was investigated by ultraviolet photoelectron spectroscopy (UPS). It was for the first time demonstrated where the intensities of the photoelectron energy distribution curves (EDC’s) for the conduction band increase with increasing Si dose, and become saturated at a certain critical Si dose where a specific peak appears at the energy corresponding to the acceptor level of Si–GaAs. The results indicate that Si atoms act as acceptors as well as donors at a high Si dose. An observation of an increasing inelastic peak height in the UPS spectrum with the Si dose also gave us an important piece of information on a degree of the crystallinity of Si–GaAs which was degraded with the Si dose.