Orthorhombic tantalum pentoxide (β-Ta2O5) monocrystalline films were deposited on epi-GaN/α-Al2O3 (0001) substrates using the metal-organic chemical vapor deposition method. The prepared films were grown along the β-Ta2O5 (001) plane. The film deposited at 850 °C exhibited the best crystalline quality and the corresponding FWHM of the XRD ω-rocking curve for β-Ta2O5 (001) plane was 1.81°. The prepared β-Ta2O5 film possessed a domain structure, and the growth mechanism was studied in detail. By the XRD Φ scan and HRTEM analyses, the in-plane epitaxial relationship of the 850 °C-prepared sample was determined as β-Ta2O5[100] ‖ GaN [1‾100]. The elemental composition and valence states were studied and the band gap of the film prepared at 850 °C was calculated to be 4.34 eV by the analysis of the electron energy loss spectrum.
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