Thesis (Ph. D.)--University of Texas at Austin, 2006. / Vita. Includes bibliographical references.

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Thesis (Ph. D.)--University of Texas at Austin, 2000. / Vita. Includes bibliographical references (leaves 178-187). Available also in a digital version from Dissertation Abstracts.

The ability of asphalt binders (bitumen) in road surfaces to self-heal after cracking is important to developing a robust transportation system that can tolerate heavy traffic and varying weather conditions. In order to develop improved binders, there is a need for noninvasive, in-situ, interface-specific methods of monitoring the kinetics, physics and chemistry of self-healing bitumen interfaces. Here the feasibility of using optical second-harmonic generation (SHG) by focused femtosecond laser pulses to monitor bitumen surfaces is demonstrated. SHG signals are observed in transmission through a sample composed of bitumen spin-coated onto a borosilicate microscope coverslip. The SHG signals are absent from uncoated coverslips, demonstrating that they originate from the bitumen layer. Further tests demonstrate that the bitumen-air surface makes the dominant contribution to the SHG signal. The SHG signal is observed to decay on a time scale comparable to typical self-healing times because of sample heating by the incident laser irradiation. Methods to control this effect by translating the sample during data acquisition are developed. Although the present results were obtained with a single incident wavelength (800 nm), they demonstrate the feasibility of probing bitumen interfaces spectroscopically with tunable light sources in order to monitor bond-specific chemical kinetics. / text

Thesis (Ph. D.)--University of Texas at Austin, 2005. / Vita. Includes bibliographical references.

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The work presented in this thesis describes an investigation into the properties and behaviour of nonlinear optical guest molecules doped into polymeric matrices. The interactions of the guest molecule 2-(N, N dimethylamino)-5-nitroacetanilide (DAN) with a polycarbonate and polymethyl methacrylate (PMMA) host are compared. A detailed characterisation of the two systems is described employing infra red spectroscopy and analysis of the chromophore alignment during electric field poling. The study reveals that hydrogen bond formation between the guest and the polar polycarbonate backbone accounts for the unusually good alignment stability previously reported in the polycarbonate system. The molecular hyperpolarisibility of DAN in PMMA is also measured and the apparent enhancement compared with solution measurements is accounted for by the more polar nature of the polymer environment. A new technique allowing the measurement of the dipole moment of polar molecules doped into thin polymer films is also presented. The technique is demonstrated on a series of zwitterionic chromophores whose measured dipole moments range from 30 to 40 D. Electrochroism measurements are performed to account for aggregation of the monomer species which then permits the first hyperpolarisibility of the molecules to be calculated. The values of dipole moment and hyperpolarisibility are found to be very sensitive to the choice of dielectric cavity shape used when deriving the local field correction factors. The measured values are therefore compared with theoretical calculations and a preferred cavity shape is proposed.

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