Kinetics versus thermodynamics of the metal incorporation in molecular beam epitaxy of (In_xGa_1−x)₂O₃

We present a detailed study of the reaction kinetics and thermodynamics of the plasma-assisted oxide molecular beam epitaxy of the ternary compound (InxGa1−x)2O3 for 0 ≤ x ≤ 1. We measured the growth rate of the alloy in situ by laser reflectrometry as a function of growth temperature TG for different metal-to-oxygen flux ratios rMe, and nominal In concentrations xnom in the metal flux. We determined ex situ the In and Ga concentrations in the grown film by energy dispersive X-ray spectroscopy. The measured In concentration x shows a strong dependence on the growth parameters TG, rMe, and xnom whereas growth on different co-loaded substrates shows that in the macroscopic regime of ∼μm3 x does neither depend on the detailed layer crystallinity nor on crystal orientation. The data unveil that, in presence of In, Ga incorporation is kinetically limited by Ga2O desorption the same way as during Ga2O 3 growth. In contrast, In incorporation during ternary growth is thermodynamically suppressed by the presence of Ga due to stronger Ga–O bonds. Our experiments revealed that Ga adatoms decompose/etch the In–O bonds whereas In adatoms do not decompose/etch the Ga–O bonds. This result is supported by our thermochemical calculations. In addition we found that a low TG and/or excessively low rMe kinetically enables In incorporation into (InxGa1−x)2O3. This study may help growing high-quality ternary compounds (InxGa1−x)2O3 allowing band gap engineering over the range of 2.7–4.7 eV.