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Off-Stoichiometry Spectroscopic Investigations of Pure Amorphous Silica and N-Doped Silica Thin Films

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Department of Molecular Sciences and Nanosystems, Ca’ Foscari University of Venice, Dorsoduro 2137, 30123 Venezia, Italy
Kyoto Institute of Technology and Research Institute for Nanoscience, Sakyo-ku, Matsugasaki 606-8585, Kyoto, Japan
§ Piezotech Japan Ltd., Sakyo-ku, Ichijouji, Mukaibata-cho 606-8126, Kyoto, Japan
Department of Chemical Sciences, University of Padua, via Marzolo 1, 35138 Padua, Italy
*E-mail: [email protected]. Phone/Fax: +81-75-724-7568.
Cite this: J. Phys. Chem. C 2013, 117, 7, 3475–3482
Publication Date (Web):January 23, 2013
https://doi.org/10.1021/jp311697g
Copyright © 2013 American Chemical Society

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    Abstract

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    Cathodoluminescence spectroscopy and X-ray photoelectron spectroscopy were concurrently used to investigate the local physicochemical nature of the amorphous lattice in pure SiO2 and N-doped SiO2 thin films prepared by radiofrequency magnetron sputtering (the latter samples deposited under a set of different conditions of N2 partial pressure). The main aim of this investigation was twofold: (i) to extend our knowledge of the physical and chemical structure of SiO2 films and (ii) to explore our capacity of manipulating, fine tuning, and measuring their stoichiometry characteristics. The presence of nitrogen atoms in the amorphous host structure was confirmed to significantly affect the formation of oxygen-deficient centers, nonbridging oxygen hole centers, and other kinds of defect complexes. The main challenge here was to relate the variations in type and concentration of these peculiar defects to the processing conditions and to the amount of nitrogen incorporated in the SiO2 amorphous matrix. The evolution of both pure and doped systems was monitored with increasing the temperature of an annealing cycle following film deposition (1 h in air, at temperatures ranging between 50 and 1200 °C, with 50 °C step). Stoichiometry changes could thus be clarified and temperature thresholds found for the annihilation of N sites and for the formation of a pseudoequilibrium stoichiometric structure in silica glass.

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    Isochronal curves of CL intensity for (a) ODC (I) and (b) NBOHC defects relating bands as a function of annealing temperature. This material is available free of charge via the Internet at http://pubs.acs.org.

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