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Gallium–indium–oxide films (GaxIn2⊟xO3), where x = 0.0–1.1, were grown by low-pressure metalorganic chemical vapor deposition using the volatile metalorganic precursors In(dpm)3 and Ga(dpm)3 (dpm = 2,2,6,6-tetramethyl-3,5-heptanedionato). The films were smooth (root mean square roughness = 50–65 Å) with a homogeneously Ga-substituted, cubic In2O3 microstructure, randomly oriented on quartz or heteroepitaxial on (100) yttria-stabilized zirconia single-crystal substrates. The highest conductivity of the as-grown films was found at x = 0.12, with σ = 700 S/cm [n-type; carrier density = 8.1 × 1019 cm⊟3; mobility = 55.2 cm2/(V s); dσ/dT<0]. The optical transmission window of such films is considerably broader than that of Sn-doped In2O3, and the absolute transparency rival or exceeds that of the most transparent conductive oxides known. Reductive annealing, carried out at 400–425 C° in a flowing gas mixture of H2 (4%) and N2, resulted in increased conductivity (σ 1400 S/cm; n-type), carrier density (1.4 × 1020 cm⊟3), and mobility as high as 64.6 cm2/(V s), with little loss in optical transparency. No significant difference in carrier mobility or conductivity is observed between randomly oriented and heteroepitaxial films, arguing in combination with other data that carrier scattering effects at high-angle grain/domain boundaries play a minor role in the conductivity mechanism.
High-quality epitaxial or highly textured NiO thin films can be grown at temperatures of 400–750°C by low-pressure metalorganic chemical vapor deposition (MOCVD) on MgO, SrTiO3, C-cut sapphire, as well as on single crystal and highly textured Ni (200) metal substrates using Ni(dpm)2 (dpm – dipivaloylmethanate) as the volatile precursor and O2 or H2O as the oxidizer/protonolyzer. X-ray diffraction (XRD), scanning electron microscopy/energy dispersive detection (SEM/EDX), and atomic force microscopy (AFM) confirm that the O2-derived NiO films are smooth and that the quality of the epitaxy can be improved by decreasing the growth temperature and/or the precursor flow rate. However, low growth temperatures (400–500 °C) lead to rougher surfaces and carbon contamination. The H2O-derived NiO films, which can be obtained only at relatively high temperatures (650–750 °C), exhibit slightly broader ω scan full width half-maximum (FWHM) values and rougher surfaces but no carbon contamination. Using H2O as the oxidizer/protonolyzer, smooth and highly textured NiO (111) films can be grown on easily oxidized single crystal and highly textured Ni (200) metal substrates, which is impossible when O2 is the oxidizer. The textural quality of these films depends on both the quality of the metal substrates and the gaseous precursor flow rate.
This communication reports rapid, efficient syntheses of the zirconium-organic metal-organic chemical vapor deposition (MOCVD) precursors Zr(acac)4 and Zr(dpm)4 (acac = acetylacetonate; dpm = dipivaloylmethanate) as well as a new, highly volatile, air- and moisture-stable Zr precursor based on a tetradentate Schiff-base ligand, Zr(tfacen)2 (tfacen = bis-trifluoroacetylacetone-ethylenediiminate). The improved one-step synthetic routes employ tetrakis(dimethylamido)zirconium as a common intermediate and represent a major advance over previous methods employing ZrCl4 or diketonate metathesis. Furthermore, Zr(tfacen)2 is shown to be an effective metal-organic precursor for the MOCVD-mediated growth of (100) oriented yttria-stabilized zirconia thin films.
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