Zinc gallate (ZnGa2O4) thin films were grown on sapphire (0001) substrate using radio frequency (RF) magnetron sputtering. After the thin film deposition process, the grown ZnGa2O4 was annealed at a temperature ranging from 500 to 900 °C at atmospheric conditions. The average crystallite size of the grown ZnGa2O4 thin films increased from 11.94 to 27.05 nm as the annealing temperature rose from 500 to 900 °C. Excess Ga released from ZnGa2O4 during thermal annealing treatment resulted in the appearance of a Ga2O3 phase. High-resolution transmission electron microscope image analysis revealed that the preferential crystallographic orientation of the well-arranged, quasi-single-crystalline ZnGa2O4 (111) plane lattice fringes were formed after the thermal annealing process. The effect of crystallite sizes and lattice strain on the width of the X-ray diffraction peak of the annealed ZnGa2O4 thin films were investigated using Williamson-Hall analysis. The results indicate that the crystalline quality of the deposited ZnGa2O4 thin film improved at higher annealing temperatures.
In this paper, we report the growth and material characteristics of ZnGa2O4 thin films on c-plane sapphire and Si(100) substrates by a radio-frequency magnetron sputtering. When deposited on sapphire, the ZnGa2O4 film showed a polycrystalline nature and a less randomly oriented, primarily with the (111), (222) and (511) planes parallel to the substrate surface. On Si(100), the ZnGa2O4 thin film was randomly oriented with (311)- and (020)-plane polycrystalline properties. Transmission electron microscopy analysis revealed that an amorphous-layer interface was formed on the Si(100) substrate and the microstructure of ZnGa2O4 became disordered. The ZnGa2O4/sapphire emitted ultraviolet photoluminescence and green emissions. The dominant optical transitions depended on the deposition temperature, oxygen and Zn contents, and nature of the substrate. The structural and optical properties of sputter-deposited ZnGa2O4 thin film on sapphire indicated that sapphire substrate is suitable for the growth of crystalline, high-quality ZnGa2O4 thin film.
ZnGa2O4 films with different nitrogen impurity concentrations were deposited using radio frequency magnetron sputtering in an ammonia (NH3)/Ar gas mixture and were post-annealed at different temperatures, ranging from 600 °C to 900 °C, in NH3 atmosphere. The influence of ammonia partial pressure ratio and nitridation temperature on the microstructure, surface morphology, nitrogen doping profile, and optical properties has been investigated. The optical band gap of ZnGa2O4, under in-situ nitrogen-doping, decreases from 4.6 to 4.1 eV but the primitive ZnGa2O4 crystalline structure does not change. On nitridation, the optical band gap gradually decreases from 4.6 to 2.1 eV and the ZnGa2O4 changes into a zinc gallium oxynitride quaternary alloy structure. Secondary ion mass spectrometry analysis revealed that nitrogen atoms were uniformly distributed in the film. The narrowing, by more than 40%, of the optical band gap is attributed to the hybridization of Zn3d and N2p orbits promote p-d repulsion in the top of the valence band, and the formation of hexagonal wurtzite phase.
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