Temperature modulation enables in situ growth of gallium oxide nanostructures on thin films exhibiting diverse morphologies

Abstract

In this study, we successfully synthesized three gallium oxide thin films on (0001)-faceted Al2O3 substrates using hydrogen-reduced chemical vapor deposition (CVD) at different deposition temperatures, resulting in distinct morphologies and crystalline phases. These films consist of two pure-phase β-Ga2O3 films and one mixed-phase film comprising both β- and ε-Ga2O3 phases. The mixed-phase samples were subsequently annealed at high temperatures to obtain pure-phase β-Ga2O3 thin films. Furthermore, by precisely controlling the growth temperature, we achieved in-situ formation of Ga2O3 nanostructures (nanowires and nanoribbons) on the surface of the β-Ga2O3 thin films. The presence of different dominant crystal planes in the samples was confirmed through X-ray diffraction analysis (XRD) for verification purposes. In directly grown β-Ga2O3 films, the (−201) plane emerged as the primary crystallographic plane, while both the (−201) and (401) planes dominated in β-Ga2O3 films obtained via ε-Ga2O3 film annealing. Raman spectroscopy findings further supported these observations regarding the crystalline phase of the films as observed through XRD analysis. Scanning electron microscopy (SEM) images revealed distinct film morphologies resulting from variations in deposition temperatures. A flatter surface was observed when a higher proportion of ε-Ga2O3 was present in the film, however, regular cracking occurred after annealing. Atomic Force Microscope (AFM) images demonstrated that at a deposition temperature of 800 °C, regular steps were present on the film's surface. Mixed-phase films exhibited hillock morphology that disappeared after annealing, leading to a decrease in the surface roughness in root mean square (RMS) value. By elevating the growth temperature, a significantly enhanced density of gallium oxide nanoribbons can be seamlessly integrated onto the film surface. The transferred nanoribbons exhibit an ultra-thin profile with a minimum thickness of merely 12 nm, rendering them more slender and economically advantageous in comparison to conventional mechanical stripping methods. This study presents a CVD-based approach for growing gallium oxide thin films with varying morphologies by employing temperature modulation and demonstrates an innovative one-step method for growing nanostructures on gallium oxide films in situ, providing valuable insights for future device development involving gallium oxide.