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An in situ second harmonic generation study of the electrochemical oxidation of silicon in fluoride media
Institution:1. Centro Universitário Christus, Street Adolfo Gurgel, 133, Cocó, Fortaleza, Ceará, Brazil;2. Universidade de Sao Paulo Faculdade de Odontologia de Ribeirao Preto, Avenue do Café – Subsector Oest- 11(N-11), Ribeirão Preto, SP, Brazil;1. Department of Physics and Astronomy, University College London, London WC1E 6BT, UK;2. Technical University of Denmark, Department of Chemical and Biochemical Engineering, Frederiksborgvej 399, 4000 Roskilde, Denmark;1. College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, 30# Puzhu South Road, Nanjing, 211816, PR China;2. Energy Engineering, Division of Energy Science, Luleå University of Technology, 97187, Luleå, Sweden;1. Université de Lorraine, LRGP, UMR 7274, Nancy, F-54001, France;2. CNRS, LRGP, UMR 7274, Nancy, F-54001, France;3. Université de Lorraine, GeoRessources, UMR 7359, Vandoeuvre-lès-Nancy, F-54506, France;4. CNRS, GeoRessources, UMR 7359, Vandoeuvre-lès-Nancy, F-54506, France;1. Natural Resources Canada, CanmetENERGY, 1 Haanel Drive, Ottawa, Ontario K1A 1M1, Canada;2. Department of Chemical and Biological Engineering, University of Ottawa, Ottawa, Ontario K1N 6N5, Canada
Abstract:The electrochemical oxidation of p-type Si in fluoride solutions has been studied by in situ second harmonic generation (SHG) with the SHG signal being recorded simultaneously with the cyclic voltammogram. The SHG signal is shown to change in tandem with the electrochemical response enabling the identification of transition points between different surface conditions such as hydrogen-terminated, hydrated oxide and oxide. Interpretation of the changes in SHG suggests that the initial response is due to the electric field-induced second harmonic (EFISH) due to the electric field gradient at the interface. It then becomes dominated by the variation in the resonant surface non-linear susceptibility as the changes in local bonding affect the response. SHG signals display a much greater sensitivity to surface conditions than the voltammetric response and allow the real-time identification of the potentials at which significant changes take place in the state of the surface.
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