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Epitaxial growth of InP single crystal thin films on (100)-oriented GaAs was tried using the molecular beam deposition method. Stoichiometric InP films have been successfully grown at the growth rate of 50 to 100 aa/min and at the substrate temperature Ts of 200=300 C under the condition of sufficient supply of P2 beams. In particular, InP films grown at Ts=240 C were evaluated to be the best by reflection high energy electron diffraction, scanning electron microscopy and electrical measurements. Epitaxial surfaces prepared by this method were several hundred times as smooth as those grown by liquid-phase or vapour-phase epitaxy, and by doping Sn into the InP films during molecular/beam epitaxy the surface morphology was greatly improved.