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On the transformation of "zincone"-like into porous ZnO thin films from sub-saturated plasma enhanced atomic layer deposition.

ABSTRACT: The synthesis of nanoporous ZnO thin films is achieved through annealing of zinc-alkoxide ("zincone"-like) layers obtained by plasma-enhanced atomic layer deposition (PE-ALD). The zincone-like layers are deposited through sub-saturated PE-ALD adopting diethylzinc and O₂ plasma with doses below self-limiting values. Nanoporous ZnO thin films were subsequently obtained by calcination of the zincone-like layers between 100-600 °C. Spectroscopic ellipsometry (SE) and X-ray diffraction (XRD) were adopted in situ during calcination to investigate the removal of carbon impurities, development of controlled porosity, and formation and growth of ZnO crystallites. The layers developed controlled nanoporosity in the range of 1-5%, with pore sizes between 0.27 and 2.00 nm as measured with ellipsometric porosimetry (EP), as a function of the plasma dose and post-annealing temperature. Moreover, the crystallinity and crystallite orientation could be tuned, ranging from a powder-like to a (100) preferential growth in the out-of-plane direction, as measured by synchrotron-radiation grazing incidence XRD. Calcination temperature ranges were identified in which pore formation and subsequent crystal growth occurred, giving insights in the manufacturing of nanoporous ZnO from Zn-based hybrid materials.

SUBMITTER: Perrotta A

PROVIDER: S-EPMC6444448 | biostudies-literature | 2019

REPOSITORIES: biostudies-literature

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Project description:This work reports the ellipsometry analysis of atomic layer deposition (ALD) films of ZnO doped with Zr to determine parameters like free carrier concentration and mobility. Thin films of zinc oxide (ZnO) and Zr-doped ZnO of thickness ∼100 nm were prepared by atomic layer deposition on sapphire, SiO2/Si(100), and Si(100) substrates. Variable-angle spectroscopic ellipsometry was used to study their optical properties in the 0.5-3.5 eV spectral range. The optical constants were accurately obtained using a model that combines Drude and Tauc-Lorentz oscillators with Bruggeman effective medium approximations, allowing the inclusion of a roughness layer in the optical model. The effect of Zr doping (ca. 1.9-4.4 atom %) was then investigated in both as-prepared samples and samples annealed in the temperature range of 100-300 °C. All of the films exhibited good optical transparency (ca. 70-90% in the visible region). For doping levels below 2.7 atom %, the real part of the dielectric permittivity reveals a semiconductor-to-metal transition in the near-infrared (NIR) region, as the permittivity goes from positive to negative. Besides, the plasma energy increases with increasing Zr concentration, and both resistivity and carrier concentration exhibit slightly parabolic behaviors, with a minimum of ∼1.5 × 10-3 Ω cm and a maximum of 2.4 × 1020 cm-3, respectively, at the same critical Zr concentration (2.7 atom %). In contrast, the carrier mobility decreases rapidly from 76.0 to 19.2 cm2/(V s) with increasing Zr content, while conductivities and carrier mobilities worsen when the annealing temperature increases, probably due to the segregation of ZnO crystals. Finally, the optical band gap is very stable, revealing its interesting independence of substrate composition and annealing temperature, as it collapses to a single master curve when band gap energy is plotted versus free carrier concentration, following the Burstein-Moss effect. Overall, the Zr-doped ZnO films studied here would be a highly desirable system for developing thermally stable transparent conductive oxides (TCOs).

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On the transformation of "zincone"-like into porous ZnO thin films from sub-saturated plasma enhanced atomic layer deposition.

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