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Using a novel two-beam technique developed to greatly enhance quadrupolar contributions to the second-order nonlinear polarization, we performed a nonlinear spectroscopic study of silicon nanocrystals implanted in an SiO₂ matrix.

Information regarding the structure and function of living tissues and cells is instrumental to the advancement of cell biology and biophysics. Nonlinear optical microscopy can provide such information, but only certain biological structures generate nonlinear optical signals. Therefore, structural specificity can be achieved by introducing labels for nonlinear optical microscopy. Few studies exist in the literature about labels that facilitate harmonic generation, coined "harmonophores". This thesis consists of the first major investigation of harmonophores for third harmonic generation (THG) microscopy. Carotenoids and chlorophylls were investigated as potential harmonophores. Their nonlinear optical properties were studied by the THG ratio technique. In addition, a tunable refractometer was built in order to determine their second hyperpolarizability (γ). At 830 nm excitation wavelength, carotenoids and chlorophylls were found to have large negative γ values however, at 1028 nm, the sign of γ reversed for carotenoids and remained negative for chlorophylls. Consequently, at 1028 nm wavelength, THG signal is canceled with mixtures of carotenoids and chlorophylls. Furthermore, when such molecules are covalently bonded as dyads or interact within photosynthetic pigment-protein complexes, it is found that additive effects with the γ values still play a role, however, the overall γ value is also influenced by the intra-pigment and inter-pigment interaction. The nonlinear optical properties of aggregates containing chlorophylls and carotenoids were the target of subsequent investigations. Carotenoid aggregates were imaged with polarization-dependent second harmonic generation and THG microscopy. Both techniques revealed crystallographic information pertaining to H and J aggregates and β-carotene crystalline aggregates found in orange carrot. In order to demonstrate THG enhancement due to labeling, cultured cells were labeled with carotenoid incorporated liposomes. In addition, Drosophila melanogaster larvae muscle as well as keratin structures in the hair cortex were labeled with β-carotene. Polarization-dependent THG studies may be particularly useful in understanding the structural organization that occurs within biological structures containing carotenoids and chlorophylls such as photosynthetic pigment-protein complexes and carotenoid aggregates in plants and alga. Further, artificial labeling with carotenoids and chlorophylls may be useful in clinical applications since they are nontoxic, nutritionally valuable, and they can aid in visualizing structural changes in cellular components.

Orbital angular momentum (OAM) is a property of light that is widely used for applications in bioimaging, optical communication and optical manipulation, but is mainly limited to the infrared and visible spectra. Developing a table-top source of Extreme Ultraviolet (XUV) light containing an arbitrary amount of OAM is yet to be achieved. We accomplish this by exploiting high-harmonic generation (HHG), a process whereby an infrared pump beam produces high order harmonics. We experimentally demonstrate the conservation of OAM in HHG by measuring harmonics of order n containing n times the OAM of the pump (n = 11, 13, 15 in our experiment). These results agree with our theoretical model. We also show theoretically how to manipulate the HHG process to impart an arbitrary amount of OAM to the di fferent harmonics. We hence show the way to a table-top and flexible source of XUV light containing orbital angular momentum.

Implementation of the ultrasonic second harmonic generation has typically been restricted to simple setups such as through-transmission or Rayleigh surface waves. Recent research has evaluated the second harmonic generation in P- and SV- waves reflected from a stress-free surface to enable the single-sided interrogation of a specimen. This research considers the second harmonic generation in an aluminum specimen, which is analytically evaluated using an approach based on the perturbation method. Here, the model is chosen to mimic an experimental setup where a longitudinal wave is generated at an oblique angle and the reflected wave is detected using a set of wedge transducers. Due to mode conversion at the interface of the wedge and the specimen, it is necessary to evaluate longitudinal and shear waves, determining all second harmonic waves generated in the bulk and at the stressfree boundary. The theoretically developed model is then implemented in a commercial finite element code, COMSOL, using increasing fundamental wave amplitudes for different values of third order elastic constants. The results of this computational model verify the analytical approach and the proposed measurement setup, taking into account assumptions and approximations of the solution procedure. Furthermore, the computational model is used to draw important conclusions relevant to the experimental setup, including the need to avoid evolving surface waves and interactions with diffracted waves. These numerical results are used to develop a recommendation for the measurement position and incident angle. Finally, the nonlinearity of two different aluminum specimens is measured with the suggested measurement setup and the results confirm the feasibility of the single-sided determination of the acoustic nonlinearity using reflected bulk waves.

Thesis (Ph. D.)--University of Texas at Austin, 2007. / Vita. Includes bibliographical references.

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

When intense laser pulses interact with an atomic or solid target, high order harmonics of the fundamental laser frequency are generated. In the case of atoms, this highly nonlinear optical process is initiated by ionization and terminated by the energetic recollision and recombination of the ionized electron with its correlated ion. In this thesis I demonstrate, both theoretically and experimentally, that high harmonics from bulk crystals can originate from the recollision of electrons with their associated holes, similarly to the atomic case, but where ionization is replaced by excitation of electron-hole pairs that accelerate within the material. This model is first derived from a quantum-mechanical theory of the solid-laser interaction, and then confirmed experimentally in ZnO and Si crystals. Despite the link I establish between high harmonic generation in solids and gases, there are notable dissimilarities. These include: a generalized motion of electrons and holes in their respective bands and its consequences, a more prominent role of dephasing and enhanced sensitivity to perturbing fields. These aspects are investigated throughout this thesis. Finally, I develop a method that exploits the recollision mechanism to reconstruct the momentum-dependent band structure of solids.

Orbital angular momentum (OAM) is a property of light that is widely used for applications in bioimaging, optical communication and optical manipulation, but is mainly limited to the infrared and visible spectra. Developing a table-top source of Extreme Ultraviolet (XUV) light containing an arbitrary amount of OAM is yet to be achieved. We accomplish this by exploiting high-harmonic generation (HHG), a process whereby an infrared pump beam produces high order harmonics. We experimentally demonstrate the conservation of OAM in HHG by measuring harmonics of order n containing n times the OAM of the pump (n = 11, 13, 15 in our experiment). These results agree with our theoretical model. We also show theoretically how to manipulate the HHG process to impart an arbitrary amount of OAM to the di fferent harmonics. We hence show the way to a table-top and flexible source of XUV light containing orbital angular momentum.