This study presents a novel approach to control the crystalline phase and surface morphology of substable ε-Ga2O3 thin films by regulating the hydrogen flow rate during chemical vapor deposition (CVD). The objective is to achieve high-quality and cost-effective heteroepitaxial pure-phase single-crystalline ε-Ga2O3 thin films on sapphire substrates. The crystalline phases and crystalline qualities of the thin films were determined by X-ray diffraction (XRD) and Raman spectroscopy. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) results show that the surface of the ε-Ga2O3 films prepared by this method is flat and the minimum value of the surface roughness (RMS) is 4.130 nm. We explain the reason for the differences in the surface morphology of the films from the point of view of hydrogen passivation. Measurements by UV–Visible spectrophotometer, the UV cut-off edge is located at 250 nm and the optical band gap is about 4.9 eV. The experimental results show that with the increase of hydrogen flow rate, the content of β-Ga2O3 in the films and the surface roughness and maximum height of the contour (RZ) decreases, until a smooth surface of the pure-phase ε-Ga2O3 film is produced. The success of the chemical vapor deposition method for heterogeneous epitaxy of high-quality ε-Ga2O3 films on sapphire substrates greatly reduces the production cost and expensive investment in production equipment, which makes its application in high electron mobility transistors, piezoelectric resonators, and sun-blind detectors have great potential, and at the same time, this method provides ideas for the preparation of other metastable materials.
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