The optical cubic susceptibility dispersion of some transparent thin films.

The aim of this dissertation has been to investigate the third order nonlinear susceptibility dispersion of molecules and polymers in order to estimate their purely electronic nonlinear response and in particular their optical Kerr nonlinear susceptibility in the 1 to 2 μm infrared spectral region. We have been successful in modeling with a four level system the near resonant cubic susceptibility of the polydiacetylene, poly(4-BCMU). In that case tunable Third-Harmonic-Generation and Two-Photon-Absorption measurements both agreed with the result of a Near-Infrared-Three-Wave-Mixing measurement. In the case of β-carotene and polythiophenes the four level model also fits the Third-Harmonic-Generation data well. In the previously mentioned cases the spectral behavior of the Two-Photon figure of merit derived by Mizrahi et al. is calculated. The four level model, when extrapolated far off resonance predicts that an all-optical switching device constructed with these materials will be dominated by Two-Photon-Absorption. A promising new class of side-chain substituted polymers with large microscopic second order nonlinearities was also investigated. Third-Harmonic-Generation measurements indicate that no forbidden two-photon transition is present in this case and that the magnitude of the nonlinear third order susceptibility is dominated by the charge-transfer nature of the nonlinear moieties combined with cascading of second order effects at a microscopic level. In the case of Sol-Gel thin films of varying TiO₂ concentration in SiO₂, the formula derived by Boling et al., based also on a three level model, predicts successfully the magnitude of the third order susceptibility. THG is in that case an invaluable technique used for the first time to measure relatively small nonlinear susceptibilities of glass-like thin films.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

doctoral

Discipline thesis:degree_discipline

Optical Sciences

Grantor dc:publisher

The University of Arizona.

Year dc:date.issued

1991

Author dc:creator

• Torruellas, William Eugene.

Advisor dc:contributor.advisor

• Stegeman, George I.

Committee members dc:contributor.committeemember

• Peyghambarian, Nasser
• Wright, Ewan M.

• Dissertations, Academic
• Chemistry, Physical and theoretical.

Statement dc:rights

• Copyright © is held by the author. Digital access to this material is made possible by the University Libraries, University of Arizona. Further transmission, reproduction or presentation (such as public display or performance) of protected items is prohibited except with permission of the author.

Language dc:language.iso

en

Handle dc:identifier.uri

http://hdl.handle.net/10150/185366

OAI identifier oai:identifier

oai:repository.arizona.edu:10150/185366