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X-ray absorption, photoemission spectroscopy, and Raman scattering analysis of amorphous tantalum oxide with a large extent of oxygen nonstoichiometry
Authors:Tsuchiya Takashi  Imai Hideto  Miyoshi Shogo  Glans Per-Anders  Guo Jinghua  Yamaguchi Shu
Institution:Department of Materials Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo, Tokyo 113-8656, Japan. tsuchiya@alto.material.t.u-tokyo.ac.jp
Abstract:The electronic structure and modification of the local interatomic structure of a reactive sputtered amorphous tantalum oxide (a-TaO(x)) thin film with the variation of oxygen nonstoichiometry, x in a-TaO(x) have been investigated by X-ray absorption spectroscopy (XAS), X-ray photoemission spectroscopy (XPS), Raman scattering spectroscopy, and Rutherford back scattering spectroscopy. A parallel chemical shift of Ta4f(7/2) and O1s core levels observed with the variation of x indicates the Fermi level shift by reduction and oxidation in the framework of the rigid band model. Extended X-ray absorption fine structure (EXAFS) suggests both the increase of average coordination number of the first Ta-O shell in polyhedra and a considerable reduction of the average Ta-O bond length with the increase of x. The relative intensity of Raman shift peaks at 670 cm(-1) and 815 cm(-1), corresponding to Ta-O stretching of TaO(6) octahedra and TaO(5) probably with a pyramidal form, respectively, drastically changes between x = 2.47 to 1.86, suggesting the change in the predominant polyhedron from TaO(6) to TaO(5) with a modification in multiplicity of oxygen by the reorganization of the polyhedral network.
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