摘要： Incorporating dissimilar semiconductors into a single platform can offer additional degrees of freedom for optoelectronic device design. However, bonding of elements with mixed valence at heterovalent interfaces often leads to defect formation and poor material quality. Using ZnSe/GaAs as a model system, we investigate the use of above-bandgap photon irradiation in combination with elemental surface treatments as a route to modify the interface properties. We find that this approach produces large changes in the behavior of the interfaces. Specifically, treating the GaAs surface with light and a short exposure to Se flux results in strong excitonic emission from both layers and an abrupt interface between them. We propose that these improvements arise from controlled desorption of As atoms from the GaAs surface and the subsequent Se enrichment of the interface. These results suggest that illumination with above-bandgap photons and proper choice of elemental exposure prior to heterovalent epitaxial layer growth may aid the synthesis of heterovalent semiconductor heterostructures.