In this study, we present a significant advance in the growth of epitaxial GeTe-Sb2Te3 alloys on Si(111)-(√3 × √3)R30°-Sb reconstructed surface by means of Molecular Beam Epitaxy. By employing X-ray diffraction and Raman spectroscopy, we show how phase, composition, and vacancy ordering can be tailored by tuning the growth parameters such as Ge and Te elemental fluxes as well as the substrate temperature. The effect of each parameter on the GeSbTe composition and phase is also discussed. A very surprising finding is that GeSbTe alloys are more ordered when grown at lower substrate temperatures. In addition, it was possible to fabricate ordered GeSbTe even for substrate temperatures as low as 120 °C. In situ high-energy electron diffraction is employed to monitor the crystallinity and surface roughness of GeSbTe films at different stages of growth. Thus, we identify the deposition parameter ranges whereby high structural quality GeSbTe with flat surfaces can be obtained.

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