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Please use this identifier to cite or link to this item: http://hdl.handle.net/1807/17741

Title: Amplified Photochemistry with Slow Photons
Authors: Chen, Jennifer I-Ling
Advisor: Ozin, Geoffrey Alan
Department: Chemistry
Keywords: slow photons
photochemistry
photonic crystal
Issue Date: 23-Sep-2009
Abstract: Slow photon, or light with reduced group velocity, is a unique phenomenon found in photonic crystals that theoreticians have long suggested to be invaluable for increasing the efficiency of light-driven processes. This thesis demonstrates experimentally the feasibility of using slow photons to optically amplify photochemistry of both organic and inorganic systems. The effect of photonic properties on organic photochemistry was investigated by tracing out the wavelength-dependent rate of photoisomerization of azobenzene anchored on silica opals. The application of slow photons to inorganic photochemical processes was realized by molding nanocrystalline titania into an inverse opal structure and investigating its photodegradation efficiency in relation to the photonic properties. Changes in the photodegradation efficiency were directly linked to modifications of the electronic band gap absorption as a result of the photonic properties. The highest enhancement of twofold was achieved when the energy of the slow photons overlaps with the electronic band gap absorption, such that the loss of light due to photonic stop-band reflection was significantly reduced. In addition, the strength of slow-photon amplification with respect to the macroscopic structural order was studied by introducing controlled disorder via the incorporation of guest spheres into the opal templates. For the first time, a correlation between structural order, photonic properties and a photochemical process was established. The ability to combine slow-photon optical amplification with chemical enhancement was further achieved by incorporating platinum nanoparticles in inverse titania opals where the platinum nanoparticles increased the lifetimes of the higher population of electron-hole pairs arising from slow photon. Overall, various important factors governing the slow photon enhancement were investigated in detail, including the energy of the photonic stop band, angle dependence, thickness of the film, degree of structural order, filling fraction of the dielectric material and diffusion of a second medium if present. Theoretical calculations based on scalar-wave approximation in support of the experimental findings were provided wherever possible. The findings provide a blueprint for achieving optical amplification using slow photons in the broad range of photochemical or photophysical processes.
URI: http://hdl.handle.net/1807/17741
Appears in Collections:Doctoral
Department of Chemistry - Doctoral theses

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