|Institution:||University of Rochester|
|Keywords:||Chiral photonic bandgap microcavities; Cholesteric and nematic liquid crystals; Confocal fluorescence microscopy; Fluorescence antibunching; Nanocrystal quantum dots and nanodiamonds; Room temperature single-photon sources|
|Full text PDF:||http://hdl.handle.net/1802/21675|
In this thesis I present experimental demonstrations of room-temperature, single-photon sources with definite linear and circular polarizations. Definite photon polarization increases the efficiency of quantum communication systems. In contrast with cryogenic-temperature single-photon sources based on epitaxial quantum dots requiring expensive MBE and nanofabrication, my method utilizes a mature liquid crystal technology, which I made consistent with single-emitter fluorescence microscopy. The structures I have prepared are planar-aligned cholesteric liquid crystals forming 1-D photonic bandgaps for circularly-polarized light, which were used to achieve definite circularly-polarized fluorescence of single emitters doped in this environment. I also used planar-aligned nematic liquid crystals to align single molecules with linear dipole moments and achieved definite linearly-polarized fluorescence. I used single nanocrystal quantum dots, single nanodiamond color-centers, rare-earth-doped nanocrystals, and single terrylene and DiIC18(3) dye molecules as emitters. For nanocrystal quantum dots I observed circular polarization dissymmetry factors as large as ge = -1.6. In addition, I observed circularly-polarized resonances in the fluorescence of emitters within a cholesteric microcavity, with cavity quality factors of up to Q ~ 250. I also showed that the fluorescence of DiIC18(3) dye molecules in planar-aligned nematic cells exhibits definite linear polarization, with a degree of polarization of p = -0.58 ± 0.03. Distributed Bragg reflectors form another type of microcavity that can be used to realize a single-photon source. I characterized the fluorescence from nanocrystal quantum dots doped in the defect layers of such microcavites, both organic and inorganic. Finally, to demonstrate the single-photon properties of single-emitter-doped cholesteric and nematic liquid crystal structures and distributed Bragg reflector microcavities, I present observations of photon antibunching from emitters doped in each of these structures. These experimental observations include photon antibunching from: nanocrystal quantum dots and nanodiamond color-centers doped in a cholesteric microcavity; terrylene and DiIC18(3) dye molecules doped in nematic structures, and nanocrystal quantum dots doped in the distributed Bragg reflector microcavity. A value of the zero-time second-order coherence as low as g(2)(0) = 0:001 ± 0.03 was measured. These results represent an important step forward in the realization of room temperature single-photon sources with definite polarization for secure quantum communication.