Short-range positional order in phase separated indium gallium oxide islands deposited in a reducing atmosphere

Abstract

We report a spontaneous phase separation in indium gallium oxide thin films with a nominal composition of (In0.006Ga0.994)2O3 grown on sapphire (0001) substrates using a powder sputtering method in a reducing atmosphere. The In-rich (In0.24Ga0.76)2O3-x domains are non-stoichiometric and located underneath the surface islands, whereas the In-poor domains are nearly stoichiometric Ga2O3, forming a continuous flat surface, though both domains have a monoclinic crystal structure. Furthermore, the In-rich domains exhibit a short-range positional order with a correlation length of approximately 1 μm because the phase separation occurs along the binodal decomposition accompanying periodic concentration profiling of In atoms. The analysis of X-ray photoelectron spectroscopy confirmed that the non-stoichiometry of the thin films originated from the formation of Ga sub-oxide (Ga2O) and metallic Ga, whereas the chemical state of the In atoms was close to In2O3 rather than metallic In. Our results indicate that the spontaneous phase separation occurs in (InxGa1-x)2O3 thin films even at an In content of 0.6 at%. Also, the non-stoichiometry associated with oxygen vacancies is an important parameter for causing spontaneous phase separation via the segregation of In atoms. © 2023 Elsevier B.V.