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Due to the S passivation, a modified growth of Co on GaAs(001) has been found. Using reflection high-energy electron diffraction and transmission electron microscopy, we observed the formation of a hcp Co overlayer of approximately 5 nm thickness on S/GaAs(001). In contrast, a similar 5 nm Co film on GaAs(001) shows a bcc structure. The metal-semiconductor interfaces in both systems were found to be different, where Co/S/GaAs(001) showed a relatively more abrupt interface. This epitaxial modification is explained on the basis of the morphology of the initial substrate surface, chemical compositions, the nature of the chemical reaction between adatoms and substrate atoms, and the effect of atomic segregation. © 2001 American Institute of Physics.