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A0.26Ga0.74N/AlN/GaN heterostructures with 1-nm-thick AlN interfacial layers were grown on 100-mm-diameter epitaxial AlN/sapphire templates and sapphire substrates by metalorganic vapor phase epitaxy (MOVPE). Very high Hall mobilities of approximately 2100 cm2/Vs at room temperature and approximately 25000 cm2/Vs at 15 K with a 2DEG density of approximately 1× 1013/cm2 were uniformly obtained for AlGaN/ AlN/GaN heterostructures on 100-mm-diameter epitaxial AIN/ sapphire templates. High-electron-mobility transistors (HEMTs) were successfully fabricated on the AlGaN/AlN/GaN film on the epitaxial AIN/sapphire template. The fabricated devices exhibited good pinch-off characteristics and a very high intrinsic transconductance of 496 mS/mm.