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The optical and electrical characteristics of zinc oxide (ZnO) films grown by molecular-beam epitaxy (MBE) on Si substrates were investigated. ZnO epitaxial layer was successfully grown on nitridated Si(100) substrate initially covered with high-temperature GaN and low-temperature ZnO double buffer layers using MBE. X-ray diffraction and photoluminescence results both indicated that a reasonable quality of ZnO epitaxial layer was obtained. As the CV measurement had indicated, the carrier concentration was reduced virtually in a linear fashion from ZnO surface down to GaN buffer layer. A reduction in electron concentration was caused by the carrier depletion due to the presence of the Schottky barrier of Ni/ZnO. The large density of electron accumulated at the ZnO/GaN interface was due to the large conduction band discontinuity and offset.