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Highly degenerate Ga‐doped Si (100) has been prepared using 4 keV liquid‐metal ion gun implantation and rapid thermal annealing, and has been studied using x‐ray photoelectron spectroscopy. Si 2p core electron measurements provide the most direct experimental evidence of annealing‐promoted tetrahedral SiGa bonds. The Ga, as high as 10 at. % after annealing at 500 °C, was found to occupy substitutional sites close to the surface. The surface concentration decreased with increasing annealing temperature. We find that the full width at half maximum of the Si 2p core levels increases with increasing substitutional Ga concentration. This can be explained by bond‐length and bond‐angle deviations of nearby SiSi bonds caused by SiGa bond formation and the resultant net static charge variations in the silicon lattice. We discuss the binding energy shift of both the Si 2p core level and the valence‐band maximum produced by SiGa bonding.