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.

No description available.

No description available.

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.

No description available.

Hui Yuen Yung. / Thesis submitted in: August 1998. / Thesis (M.Phil.)--Chinese University of Hong Kong, 1999. / Includes bibliographical references (leaves 70-73). / Text in English; abstract also in Chinese. / Hui Yuen Yung. / Acknowledgements --- p.vi / Abstract --- p.vii / Chapter 1 --- Introduction --- p.1 / Chapter 2 --- Second harmonic generation --- p.5 / Chapter 2.1 --- Introduction --- p.5 / Chapter 2.2 --- Maxwell's equations in dielectric media --- p.6 / Chapter 2.3 --- Second harmonic generation --- p.7 / Chapter 2.4 --- Phase matching --- p.8 / Chapter 2.5 --- Quasi phase matching --- p.10 / Chapter 2.6 --- Inversion symmetry --- p.11 / Chapter 3 --- Third order nonlinear optical processes in optical fibers --- p.14 / Chapter 3.1 --- Introduction --- p.14 / Chapter 3.2 --- Optical fibers --- p.15 / Chapter 3.3 --- Third order interaction between waves of same frequency --- p.16 / Chapter 3.4 --- Third order interaction between waves of different frequencies --- p.19 / Chapter 4 --- Multiphoton ionization interference effect --- p.23 / Chapter 4.1 --- Historical development --- p.23 / Chapter 4.2 --- Multiphoton ionization interference effect --- p.26 / Chapter 4.3 --- Periodic ionization --- p.27 / Chapter 4.4 --- Periodic electric field --- p.28 / Chapter 4.5 --- Physical interpretation --- p.29 / Chapter 5 --- Experimental setup --- p.32 / Chapter 5.1 --- Introduction --- p.32 / Chapter 5.2 --- Laser system --- p.32 / Chapter 5.3 --- Optical fibers --- p.33 / Chapter 5.4 --- Coupling light into fibers --- p.34 / Chapter 5.5 --- Detection system --- p.36 / Chapter 5.6 --- Optical layout --- p.36 / Chapter 6 --- Second harmonic generation in optical fibers --- p.40 / Chapter 6.1 --- Introduction --- p.40 / Chapter 6.2 --- Self-preparation in optical fibers --- p.41 / Chapter 6.3 --- Polarization dependence --- p.42 / Chapter 6.4 --- Seeding optical fibers --- p.42 / Chapter 6.5 --- Seeding by varying green light intensity --- p.45 / Chapter 6.6 --- Square dependence of second harmonic generation in optical fibers --- p.46 / Chapter 7 --- Erasure of x(2) grating in optical fibers --- p.56 / Chapter 7.1 --- Introduction --- p.56 / Chapter 7.2 --- Experiment --- p.58 / Chapter 7.3 --- Results --- p.59 / Chapter 7.3.1 --- Erasure by different propagating mode --- p.59 / Chapter 7.3.2 --- Erasure in germanium-doped fiber --- p.60 / Chapter 7.3.3 --- Erasure in erbium-doped fiber --- p.61 / Chapter 7.4 --- Discussion --- p.61 / Chapter 8 --- Conclusion --- p.68 / Chapter 8.1 --- Summary of our work --- p.68 / Chapter 8.2 --- Outlook --- p.69 / Chapter 8.2.1 --- Multiphoton ionization in polymer --- p.69 / Chapter 8.2.2 --- Erasure by blue light --- p.69 / Bibliography --- p.70

Choy Kwok Wai = 利用全光極化在本體聚合物中產生準相匹配二次諧波 / 蔡國偉. / Thesis submitted in: August 2005. / Thesis (M.Phil.)--Chinese University of Hong Kong, 2006. / Includes bibliographical references (leaves 132-133). / Text in English; abstracts in English and Chinese. / Choy Kwok Wai = Li yong quan guang ji hua zai ben ti ju he wu zhong chan sheng zhun xiang pi pei er ci xie bo / Cai Guowei. / Acknowledgements --- p.ii / Abstract --- p.iii / Chinese Abstract --- p.V / Table of Contents --- p.vi / List of Figures --- p.ix / Chapter Chapter 1 --- Introduction --- p.1 / Chapter 1.1 --- Principle and origin of nonlinear optics --- p.2 / Chapter 1.2 --- Tensor properties and Inversion symmetry --- p.3 / Chapter 1.3 --- Relationship between microscopic and macroscopic nonlinear susceptibility for a poled polymer --- p.5 / Chapter 1.4 --- Second Harmonic Generation by nonlinear polarization --- p.7 / Chapter 1.5 --- Outline of the thesis --- p.9 / Figures --- p.10 / Chapter Chapter 2 --- Poling and relaxation of nonlinear optical polymeric systems --- p.11 / Chapter 2.1 --- Guest-Host nonlinear optical polymeric systems --- p.11 / Chapter 2.2 --- Poling techniques --- p.13 / Chapter 2.2.1 --- Thermal-assisted Electric Poling --- p.13 / Chapter 2.2.2 --- Photo-assisted Electric Poling --- p.15 / Chapter 2.2.3 --- All-optical Poling --- p.17 / Chapter 2.3 --- Quasi-phase-matching in bulk polymers by All-optical Poling --- p.20 / Chapter 2.4 --- Photorefractive effect in polymers --- p.22 / Chapter 2.5 --- Relaxation study of NLOP system --- p.23 / Figures --- p.27 / Chapter Chapter 3 --- Experimental Method --- p.33 / Chapter 3.1 --- Experimental Setup --- p.33 / Chapter 3.1.1 --- Laser system --- p.33 / Chapter 3.1.2 --- Data acquisition system --- p.34 / Chapter 3.1.3 --- Reference arm --- p.34 / Chapter 3.1.4 --- Optical Path --- p.35 / Chapter 3.2 --- Sample Preparation --- p.36 / Chapter 3.2.1 --- Polymer Films Preparation --- p.36 / Chapter 3.2.2 --- Bulk Polymers Preparation --- p.38 / Chapter 3.3 --- Poling and Thermal history of samples --- p.41 / Figures --- p.43 / Chapter Chapter 4 --- Growth and decay of optical nonlinearity in all-optically poled polymers --- p.53 / Chapter 4.1 --- Poling profiles for DR-1 and DANS doped bulk polymer by All-optical poling --- p.53 / Chapter 4.1.1 --- Poling profiles for DR-1 doped bulk polymer and polymer films by All-optical poling --- p.53 / Chapter 4.1.2 --- Possibilities of degradation of the samples during the experiment --- p.56 / Chapter 4.1.3 --- Effects of probing beam intensity and the duration of probing on the growth and decay of X(2) --- p.57 / Chapter 4.1.4 --- Poling profiles for DANS doped bulk polymer by All-optical poling --- p.57 / Chapter 4.2 --- Dependence of the poling profiles on various parameters in all-optical poling --- p.59 / Chapter 4.2.1 --- Dependence on the temperature --- p.59 / Chapter 4.2.2 --- Dependence on the relative intensities between the two seeding beams --- p.60 / Chapter 4.2.3 --- Dependence on the relative phase between the two seeding beams --- p.64 / Chapter 4.2.4 --- Tensorial properties of X(2) --- p.67 / Chapter 4.2.5 --- Dependence on the thickness of the sample --- p.68 / Chapter 4.3 --- Comparison of different relaxation models --- p.69 / Figures --- p.71 / Chapter Chapter 5 --- Growth and decay of optical nonlinearity in poled polymers with charge-generating additives --- p.89 / Chapter 5.1 --- Orientational enhancement in NLOP systems --- p.89 / Chapter 5.2 --- Space-charge field by charge-transporting molecules and sensitizer --- p.89 / Chapter 5.3 --- Poling profile of the bulk DR-1 polymer with charge-generating ingredients --- p.91 / Chapter 5.4 --- Poling profile of the bulk DANS polymer with the presence of charge-transporting molecules and sensitizers --- p.100 / Figures --- p.107 / Chapter Chapter 6 --- Growth and decay of optical nonlinearity in a nano-structured composite system --- p.113 / Chapter 6.1 --- Historical background --- p.113 / Chapter 6.2 --- Preparation of the composites films --- p.116 / Chapter 6.2.1 --- Preparation of the silver nano-particles --- p.116 / Chapter 6.2.2 --- Preparation of the composite films --- p.117 / Chapter 6.3 --- Poling profiles of polymer films with silver nano-particles --- p.118 / Figures --- p.124 / Chapter Chapter 7 --- Conclusions --- p.129 / References --- p.132

Optical second harmonic generation (SHG) is a nonlinear process that converts two photons of frequency w to a single photon of frequency 2w. In the electricdipole approximation, this process requires a noncentrosymmetric medium. For thin films present at the interface between two centrosymmetric media¡Ðsuch as the interface between two liquids, the interface between a liquid and air, or for the surface of a variety of insulators and semiconductors¡Ðonly the molecules which participate in the asymmetry of the interface contribute to the SHG. Surface SGH from molecules which exhibit a large nonlinear optical response at a specific wavelength can be used to measure the relative surface coverage of molecules at the interface as a function of the external electrochemical parameters. The polarization dependence of the surface SHG can be used to estimate the average molecular orientation of chromophores at the liquid/liquid electrochemical interface. The potential dependence of the SHG from the interface provides important information on the position of the adsorbed chromophores with respect to the interface.