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Strain relaxation at the lattice mismatched CdS/GaAs (100) interface has been investigated by reflection high‐energy electron diffraction (RHEED) and Raman scattering. In‐situ RHEED measurements indicate a gradual relief of the mismatch strain once the critical film thickness is exceeded. After‐growth Raman measurements reveal that the strain profile measured by RHEED remains ‘‘frozen’’ in the grown layer except very close to the CdS/GaAs interface, where further relaxation takes place. A microscopic calculation shows that the presence of nonuniform strain leads to phonon confinement effects, as localized modes appear in regions of similar strains.