Abstract
In this study, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and electron energy loss spectroscopy (EELS) were used to investigate in-air oxidation of silicon nanoparticles ca. 11 nm in diameter. Particle samples were prepared first by extracting them from an RF plasma synthesis reactor, and then heating them in an inert carrier gas stream. The resulting particles had varying surface hydrogen coverages and relative amounts of SiH x (x = 1, 2, and 3), depending on the temperature to which they had been heated. The particles were allowed to oxidize in-air for several weeks. FTIR, XPS, and EELS analyses that were performed during this period clearly establish that adsorbed hydrogen retards oxidation, although in complex ways. In particular, particles that have been heated to intermediate hydrogen coverages oxidize more slowly in air than do freshly generated particles that have a much higher hydrogen content. In addition, the loss of surface hydride species at high processing temperatures results in fast initial oxidation and the formation of a self-limiting oxide layer. Analogous measurements made on deuterium-covered particles show broadly similar behavior; i.e., that oxidation is the slowest at some intermediate coverage of adsorbed deuterium.
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Acknowledgments
The authors thank Bing Lou and Ozan Ugurlu for their help in analysis. This study was supported partially by the MRSEC Program of the National Science Foundation under award number DMR-0819885 and partly by the National Science Foundation under award number CHE-0924431. Parts of this study were carried out at the Institute of Technology Characterization Facility, the University of Minnesota, which has received capital equipment funding from the NSF through the MRSEC, ERC, and MRI programs.
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Winters, B.J., Holm, J. & Roberts, J.T. Thermal processing and native oxidation of silicon nanoparticles. J Nanopart Res 13, 5473 (2011). https://doi.org/10.1007/s11051-011-0535-4
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DOI: https://doi.org/10.1007/s11051-011-0535-4