The local Zn/Se relative concentration at the interface in ZnSe-GaAs(001) heterostructures synthesized by molecular beam epitaxy was found to be controlled by the Zn/Se Aux ratio employed during the early growth stage of ZnSe on GaAs. Correspondingly, the valence band discontinuity varies from 1.20 eV (Zn-rich interface) to 0.58 eV (Se-rich interface). Comparison with the results of firstprinciples calculations suggests that the observed trend in band offsets is related to the establishment of neutral interfaces with different atomic configurations.
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