Porous silicon (PSi) photonic crystals have aroused research interest as label-free chemical and biological sensing transducers owing to the ease of fabrication, high quality optics and a sensitive optical response to changes in efractive index. A major impediment to using PSi materials as sensors is the relative instability of the silicon surface to oxidation in ambient air and aqueous environments. This thesis reports methods for derivatising PSi towards realisation of 1-D silicon-based photonic materials for applications in biology and medicine. Narrow-linewidth rugate filters, a class of photonic crystal, are fabricated on silicon to display a high reflectivity resonant line in the reflectance spectrum. The position of the resonance is sensitive to changes in refractive index, thus allowing quantification of infiltrating biological species. The efficacy of rugate filters as biosensing transducers requires 1) protection from aqueous degradation, 2) resistance to non-specific adsorption and 3) distal reactivity for coupling of biorecognition molecules. Two chemical strategies based on hydrosilylation of functional alkenes are compared for stabilising the PSi structure against oxidation whilst resisting non-specific adsorption of biomolecules. Immobilisation of peptides to the organic layers is demonstrated for optical detection of protease enzymes. Introduction of protease results in cleavage of the immobilised peptides within the rugate filters, detected by an optical blue-shift to shorter wavelengths. To increase the sensitivity to proteolysis, covalent mmobilisation of biopolymers is evaluated using gelatin as a model substrate. Digestion of gelatin is detected down to 37 attomoles of protease. Furthermore, the surface chemistry allows specific capture of live cells and incubation with stimulated macrophages in tissue culture results in optical detection of released gelatinase enzymes. The generality of the surface chemistry allows for a range of other biological applications to be investigated. An alternative biorecognition interface, hybrid lipid bilayer membranes, containing specific recognition elements for cholera toxin allows optical detection of affinity capture and concentration within the PSi. In addition, the suitability of chemically modified photonic crystals as reservoirs for mass spectrometry is evaluated towards biomolecule quantification after optical detection. A robust and flexible surface chemistry on PSi photonic crystals is critical to performance in a range of biological assays and a necessary requirement for wide-scale employment.
| Identifer | oai:union.ndltd.org:ADTP/215544 |
| Date | January 2007 |
| Creators | Kilian, Kristopher, Chemistry, Faculty of Science, UNSW |
| Source Sets | Australiasian Digital Theses Program |
| Language | English |
| Detected Language | English |
| Rights | http://unsworks.unsw.edu.au/copyright, http://unsworks.unsw.edu.au/copyright |
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