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Heteroepitaxial growth of InP on Si with an intermediate GaAs buffer layer by low‐pressure organometallic vapor phase epitaxy is reported. Excellent crystallinity of InP epilayers with specular surfaces can be reproducibly obtained. The carrier concentration profile shows that the carrier distribution in the InP layer is very uniform, while an apparent reduction in concentration occurs at the InP/GaAs interface. The 77 K photoluminescence (PL) of the InP layer exhibits a strong near‐band‐edge emission. No evident shift in PL peak energy for the InP/GaAs/Si sample compared with that for the InP homoepitaxial sample was first observed in this study. These results are superior to those reported previously for the InP/Si heteroepitaxy.