The relaxation of strain in the ZnS epilayers grown on (100) GaP was investigated with resonant Raman scattering measurement. The single LO phonon resonant Raman shift and the intensity increased but the full width at half maximum decreased with the increasing ZnS epilayer thickness. These were attributed to the relaxation of the biaxial tensile strain with the generating misfit dislocations. Finally, the critical thickness of ZnS/GaP epilayer was found to be around 35 nm.
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