The nonlinear optical (NLO) properties were investigated in various extended π-conjugated chromophores: cyanine and alkyne carbocations; porphyrin dimers; and squaraine compounds that possess electronic, double resonance, and vibronic based NLO properties. In summary: (i) It was demonstrated that the alkyne carbocations have very similar optical properties to traditional cyanine dyes. Our theoretical results establish that the alkyne carbocations, in spite of their significant degree of bond-length alternation, behave in the same way as cyanine dyes. (ii) The nature of the -bridge in porphyrin dimers tunes the electronic coupling strength, which in turn determines the splitting of the energy levels and the (non)linear optical properties. (iii) We have shown that the origin of the lowest TPA-active states in squaraines is dependent on the nature of substituent donor moiety, changing from predominantly electronic to vibronic in character. For all squaraines containing indolinylidenemethyl donors, a vibronic origin for the TPA peak, and the energy and lineshape of the experimentally observed lowest TPA peak in these compounds were confirmed.
| Identifer | oai:union.ndltd.org:GATECH/oai:smartech.gatech.edu:1853/29717 |
| Date | 18 June 2009 |
| Creators | Ohira, Shino |
| Publisher | Georgia Institute of Technology |
| Source Sets | Georgia Tech Electronic Thesis and Dissertation Archive |
| Detected Language | English |
| Type | Dissertation |
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