Both hexagonal and tetragonal forms of MoSi2 (h‐MoSi2 and t‐MoSi2) were grown epitaxially on (111)Si for the first time. The best epitaxy was obtained in samples annealed at 1050 °C for 1 h. The orientation relationships between epitaxial h‐MoSi2 and Si were determined to be [0001]MoSi2//[111]Si and (202̄0)MoSi2//(202̄)Si whereas those between epitaxial t‐MoSi2 and Si were analyzed to be [110]MoSi2//[111]Si and (004)MoSi2//(2̄02)Si. Regular interfacial dislocations, 100 Å in spacing, were identified to be of edge type with (1)/(6) 〈112〉 Burgers vectors. Preliminary investigations indicated that a number of other technologically important refractory silicides can all be grown epitaxially on silicon. The results present an exciting prospect to fabricate novel classes of devices with desirable characteristics.

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