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Photoluminescence and Patterning of Silicon Nanocrystals Open Access


Other title
Size distribution
Silicon Nanocrystals
Block copolymer patterning
Type of item
Degree grantor
University of Alberta
Author or creator
Rodriguez Nunez, Jose R.
Supervisor and department
Veinot, Jonathan G. C. (Chemistry)
Examining committee member and department
Moffitt, Matthew (Chemistry, University of Victoria)
Bergens, Steven H. (Chemistry)
Meldrum, Alkiviathes (Physics)
Harrison, Jed (Chemistry)
Mar, Arthur (Chemistry)
Department of Chemistry

Date accepted
Graduation date
Doctor of Philosophy
Degree level
Silicon nanocrystals (Si-NCs) have been suggested for sensing and lasing applications due to their low-toxicity and compatibility with existing microelectronic technologies. Their broad luminescence, due to homogeneous (150 meV or 40 nm at room temperature) and inhomogeneous broadening, may hamper their incorporation into the aforementioned applications. This thesis begins with a discussion on the optical properties of Si-NCs (Chapter one). Then, it presents methods to decrease the breadth of the luminescence obtained upon photoexcitation of Si-NCs prepared via thermal processing of hydrogen silsesquioxane (HSQ). Narrowing of luminescence profile can be accomplished by sensitization of sharply emissive species. Chapter two outlines a solution processable method to obtain sharp, Si-NC sensitized, erbium luminescence. The luminescence obtained (FWHM Er emission ~ 40 nm) lies in the low-loss window of silica fiber optics and may be useful for telecommunication applications. A method to pattern oxide-embedded Si-NCs using amine containing block copolymers is presented in Chapter 3. This method utilizes gelation of HSQ with amine moieties in the polymer. This straightforward, inexpensive, non-lithographic, patterning technique was also extended to germanium features. Chapter four presents a photo-assisted etching method of Si-NCs. This unique etching method provides a means to control the optical properties of Si-NCs by exposing a Si-NC:HF:HCl mixture to light of varying wavelengths. The narrowest luminescence obtained using this technique is approximately 80 nm (twice the width of homogeneously broadened NCs). A method to prepare Si-NC coated microcavities is presented in Chapter five. The coupling of NC luminescence to optical cavities produces high quality, whispering-gallery modes which results in sharp peaks (FWHM < 0.5 nm) over the broad PL spectrum. A proof-of-concept refractometric sensor using these cavities is also discussed. Finally, Chapter 6 includes general conclusions on the work presented and outlines new research that can be performed to enable incorporation of these materials into everyday technologies.
Permission is hereby granted to the University of Alberta Libraries to reproduce single copies of this thesis and to lend or sell such copies for private, scholarly or scientific research purposes only. Where the thesis is converted to, or otherwise made available in digital form, the University of Alberta will advise potential users of the thesis of these terms. The author reserves all other publication and other rights in association with the copyright in the thesis and, except as herein before provided, neither the thesis nor any substantial portion thereof may be printed or otherwise reproduced in any material form whatsoever without the author's prior written permission.
Citation for previous publication
Rodriguez Núñez, J. R.; Bianucci, P.; Meldrum, A.; Veinot, J.G.C.; “Whispering gallery modes in hollow cylindrical microcavities containing silicon nanocrystals”, Applied Physics Letters, 92, 2008, 131119-131121Bianucci, P.; Rodriguez, J.R.; Clements, C.M.; Veinot, J.G.C.; Meldrum, A. “Silicon nanocrystal luminescence coupled to whispering gallery modes in optical fibers”. Journal of Applied Physics, 105, 2009, 231081 – 231085.Rodriguez, J.R.; Veinot, J.G.C. “Realization of sensitized erbium luminescence in Si-nanocrystal composites obtained from solution processable sol-gel derived materials”. Journal of Materials chemistry. 2010, 1713-1720Rodríguez Núñez, J. R.; Johnson, M.; Veinot, J. G. C. “Non-lithographic Patterning of Oxide Embedded Silicon Nanostructures” MRS Proceedings, 1359, Published online with no page numbers (6 pages).Rodríguez Núñez, J. R.; Kelly, J. A.; Henderson, E. J.; Veinot J. G. C. “Wavelength-Controlled Etching of Silicon Nanocrystals” Chemistry of Materials., 2012. (accepted)

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