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In this work, we show the heteroepitaxial growth of single-crystallinebixbyite (In$_{1-x}$Ga$_x$)$_2$O$_3$ films on (111)-oriented yttria-stabilizedzirconia substrates using plasma-assisted molecular beam epitaxy under variousgrowth conditions. A pure In$_2$O$_3$ buffer layer between the substrate and(In$_{1-x}$Ga$_x$)$_2$O$_3$ alloy is shown to result in smoother film surfacesand significantly improved crystallinity. Symmetric out-of-plane 2$\theta -\omega$ x-ray diffraction scans show a single (111) crystal orientation andtransmission electron microscopy confirms the single-crystallinity up to $x =0.18$ and only slight film quality deterioration with increasing Ga content.Partially relaxed layers are demonstrated via reciprocal space mapping withlattice parameters fitting well to Vegard's law. However, the Ga cations arenot evenly distributed within the films containing nominally $x > 0.11$:inclusions with high Ga density up to $x = 0.50$ are observed within a "matrix"with $x \approx 0.08$. The cubic bixbyite phase is preserved, in both the"matrix" and the inclusions. Moreover, for $x \geq 0.11$, both the Raman phononlines as well as the optical absorption onset remain nearly constant. Hardx-ray photoelectron spectroscopy measurements also indicate a widening of theband gap and exhibit similar saturation of the Ga 2p core level position forhigh Ga contents. This saturation behavior of the spectroscopic propertiesfurther supports the limited Ga incorporation into the "matrix" of the film.

physical review materials

Molecular beam epitaxy of single-crystalline bixbyite  (In$_{1-x}$Ga$_x$)$_2$O$_3$ films ($x \leq 0.18$): Structural properties and  consequences of compositional inhomogeneity