Thesis (Ph. D.)--University of Washington, 2007. / Vita. Includes bibliographical references (leaves 113-123).

Thesis (PH. D.)--Michigan State University. Chemistry, 2008. / Title from PDF t.p. (viewed on Sept. 8, 2009) Includes bibliographical references (p. 134-148). Also issued in print.

Thesis (Ph. D.)--Ohio State University, 2006. / Title from first page of PDF file. Includes bibliographical references (p. 153-159).

Semiconductors provide an interesting platform for studying light-matter interactions due to their unique electrically conductive behavior which can be deliberately altered in useful ways with the controlled introduction of confinement and doping, which changes the electronic band structure. This area of research has led to many important fundamental scientific discoveries that have in turn spawned a plethora of applications in areas such as photonics, microscopy, single-photon sources, and metamaterials. Silicon is the prevalent semiconductor platform for microelectronics because of its cost and electrical properties, while III-V materials are optimal for optoelectronics because of the ability to engineer a direct bandgap and create versatile heterojunctions by growing binary, ternary, or quaternary compounds.

O desenvolvimento da fotônica integrada vem recebendo muita atenção nos últimos anos. Sua alta funcionalidade e velocidade de transmissão de sinais possibilitam a aplicação em diversas áreas, que vão desde comunicações até biologia. O uso de polímeros em circuitos fotônicos integrados tem se mostrado interessante, pois compostos orgânicos podem ser facilmente incorporados a matrizes poliméricas. Isso faz com que as propriedades físicas do polímero possam ser modificadas de acordo com os materiais incorporados. Além disso, a técnica da fotopolimerização por absorção de dois fótons torna possível a produção de microestruturas poliméricas tridimensionais com alta resolução. A incorporação dessas microestruturas a circuitos fotônicos pode trazer um novo ramo de funcionalidades devido à facilidade de modificação das propriedades dos polímeros. Além disso, a tridimensionalidade das estruturas permite a realização de conexões ópticas em três dimensões, o que colabora para o aumento da compacticidade dos dispositivos fotônicos. No entanto, para que estas microestruturas possam ser efetivamente incorporadas aos circuitos fotônicos é necessário desenvolver formas de conectá-las a fontes externas de excitação, bem como a instrumentos de análise de sinais. Os tapers de fibras ópticas, também conhecidos como microfibras ou nanofibras, são bons candidatos para realizar essa tarefa devido a suas dimensões reduzidas, as quais são compatíveis com o tamanho das microestruturas. Neste trabalho desenvolvemos métodos para realizar a conexão óptica entre microestruturas poliméricas e tapers de fibras ópticas. As microestruturas foram produzidas através da técnica de fotopolimerização por absorção de dois fótons e corantes orgânicos foram incorporados à matriz polimérica para conferir propriedades fluorescentes às estruturas. Os tapers foram produzidos a partir de fibras ópticas convencionais por uma técnica de aquecimento e estiramento. Para realizar a conexão óptica, dois métodos foram desenvolvidos. No primeiro deles as microestruturas foram excitadas através de uma lente objetiva e sua emisão foi coletada por um taper. No segundo método, tanto a excitação quanto a coleta foram realizadas por tapers de fibras ópticas. Em ambos os casos as fibras foram posicionadas através de micromanipuladores. Os resultados obtidos indicam que os tapers são ferramentas adequadas para realizar tanto a excitação quando a coleta da emissão de microestruturas, pois permitem excitação individual e coleta localizada. Produzimos microestruturas com múltiplas dopagens e pudemos concluir que a excitação localizada de diferentes partes da estrutura, bem como a correta escolha do comprimento de onda de excitação, são mecanismos que levam a alterações no espectro de emissão, o que torna estas estruturas candidatas a fontes de luz sintonizáveis que podem ser incorporadas a dispositivos on-chip. Por fim, desenvolvemos um método de produção de microestruturas conectadas a tapers. Este trabalho abre caminho para a incorporação de microestruturas poliméricas a circuitos fotônicos e demonstra que tapers de fibras ópticas são ferramentas eficientes para a realização de microconexões ópticas. / The development of integrated photonics has received a great deal of attention in the last few years. Its high functionality and signal transmission speed allow applications in several fields, from telecommunications to biology. The use of polymeric platforms in integrated photonic circuits is interesting because organic compounds can be easily incorporated to polymeric matrixes, which makes it easy to change the physical properties of the polymer according to the embed materials. Furthermore, the two-photon polymerization technique allows the production of three-dimensional polymeric microstructures with high resolution. The incorporation of these microstructures to photonic circuits paves the way for a new field of funcionalities due to the ease of modification of the polymers properties. Besides that, the structures three-dimensionality allows the performance of optical connections in three dimensions, which can improve the compacticity of the photonic devices. However, for the effective incorporation of these microstructures to photonic circuits, it is necessary to develop ways to connect them to external excitation sources, as well as analysis instruments. Optical fiber tapers, also known as microfibers or nanofibers, are good candidates for this task due to their reduced dimensions that are compatible with the size of the microstructures. In this work we developed methods for the performance of optical connections of polymeric microstructures through fiber tapers. The microstrutures were produced through the two-photon polymerization technique and organic dyes were incorporated to the polymeric matrix in order to introduce fluorescent properties. The fiber tapers were produced from conventional optical fibers through a heat-and-draw approach. To perform the optical connections, two methods were developed. In the first one, the microestructures were excited through a microscope objective and emission collection was performed by a fiber taper. In the second approach, excitation and collection were performed by fiber tapers. In both methods, the tapers were set up by micromanipulators. The obtained results indicate that tapers are a suitable tool to perform optical excitation and emission collection in microstructures, as they allow individual excitation and localized collection. Multiple doped microstructures were produced and we could imply that the localized excitation of different parts of the structures, as well as the correct choice of the excitation wavelength, are tools that lead to changes in the emission spectrum, which makes these structures candidates to tunable light sources that can be incorporated to on-chip devices. At last, we developed a method for the production of microstructures connected to fiber tapers. This work paves the way for the incorporation of polymeric microstructures to photonics circuits and demonstrates that fiber tapers are efficient tools to perform optical microconnections.

O desenvolvimento da fotônica integrada vem recebendo muita atenção nos últimos anos. Sua alta funcionalidade e velocidade de transmissão de sinais possibilitam a aplicação em diversas áreas, que vão desde comunicações até biologia. O uso de polímeros em circuitos fotônicos integrados tem se mostrado interessante, pois compostos orgânicos podem ser facilmente incorporados a matrizes poliméricas. Isso faz com que as propriedades físicas do polímero possam ser modificadas de acordo com os materiais incorporados. Além disso, a técnica da fotopolimerização por absorção de dois fótons torna possível a produção de microestruturas poliméricas tridimensionais com alta resolução. A incorporação dessas microestruturas a circuitos fotônicos pode trazer um novo ramo de funcionalidades devido à facilidade de modificação das propriedades dos polímeros. Além disso, a tridimensionalidade das estruturas permite a realização de conexões ópticas em três dimensões, o que colabora para o aumento da compacticidade dos dispositivos fotônicos. No entanto, para que estas microestruturas possam ser efetivamente incorporadas aos circuitos fotônicos é necessário desenvolver formas de conectá-las a fontes externas de excitação, bem como a instrumentos de análise de sinais. Os tapers de fibras ópticas, também conhecidos como microfibras ou nanofibras, são bons candidatos para realizar essa tarefa devido a suas dimensões reduzidas, as quais são compatíveis com o tamanho das microestruturas. Neste trabalho desenvolvemos métodos para realizar a conexão óptica entre microestruturas poliméricas e tapers de fibras ópticas. As microestruturas foram produzidas através da técnica de fotopolimerização por absorção de dois fótons e corantes orgânicos foram incorporados à matriz polimérica para conferir propriedades fluorescentes às estruturas. Os tapers foram produzidos a partir de fibras ópticas convencionais por uma técnica de aquecimento e estiramento. Para realizar a conexão óptica, dois métodos foram desenvolvidos. No primeiro deles as microestruturas foram excitadas através de uma lente objetiva e sua emisão foi coletada por um taper. No segundo método, tanto a excitação quanto a coleta foram realizadas por tapers de fibras ópticas. Em ambos os casos as fibras foram posicionadas através de micromanipuladores. Os resultados obtidos indicam que os tapers são ferramentas adequadas para realizar tanto a excitação quando a coleta da emissão de microestruturas, pois permitem excitação individual e coleta localizada. Produzimos microestruturas com múltiplas dopagens e pudemos concluir que a excitação localizada de diferentes partes da estrutura, bem como a correta escolha do comprimento de onda de excitação, são mecanismos que levam a alterações no espectro de emissão, o que torna estas estruturas candidatas a fontes de luz sintonizáveis que podem ser incorporadas a dispositivos on-chip. Por fim, desenvolvemos um método de produção de microestruturas conectadas a tapers. Este trabalho abre caminho para a incorporação de microestruturas poliméricas a circuitos fotônicos e demonstra que tapers de fibras ópticas são ferramentas eficientes para a realização de microconexões ópticas. / The development of integrated photonics has received a great deal of attention in the last few years. Its high functionality and signal transmission speed allow applications in several fields, from telecommunications to biology. The use of polymeric platforms in integrated photonic circuits is interesting because organic compounds can be easily incorporated to polymeric matrixes, which makes it easy to change the physical properties of the polymer according to the embed materials. Furthermore, the two-photon polymerization technique allows the production of three-dimensional polymeric microstructures with high resolution. The incorporation of these microstructures to photonic circuits paves the way for a new field of funcionalities due to the ease of modification of the polymers properties. Besides that, the structures three-dimensionality allows the performance of optical connections in three dimensions, which can improve the compacticity of the photonic devices. However, for the effective incorporation of these microstructures to photonic circuits, it is necessary to develop ways to connect them to external excitation sources, as well as analysis instruments. Optical fiber tapers, also known as microfibers or nanofibers, are good candidates for this task due to their reduced dimensions that are compatible with the size of the microstructures. In this work we developed methods for the performance of optical connections of polymeric microstructures through fiber tapers. The microstrutures were produced through the two-photon polymerization technique and organic dyes were incorporated to the polymeric matrix in order to introduce fluorescent properties. The fiber tapers were produced from conventional optical fibers through a heat-and-draw approach. To perform the optical connections, two methods were developed. In the first one, the microestructures were excited through a microscope objective and emission collection was performed by a fiber taper. In the second approach, excitation and collection were performed by fiber tapers. In both methods, the tapers were set up by micromanipulators. The obtained results indicate that tapers are a suitable tool to perform optical excitation and emission collection in microstructures, as they allow individual excitation and localized collection. Multiple doped microstructures were produced and we could imply that the localized excitation of different parts of the structures, as well as the correct choice of the excitation wavelength, are tools that lead to changes in the emission spectrum, which makes these structures candidates to tunable light sources that can be incorporated to on-chip devices. At last, we developed a method for the production of microstructures connected to fiber tapers. This work paves the way for the incorporation of polymeric microstructures to photonics circuits and demonstrates that fiber tapers are efficient tools to perform optical microconnections.

New generations of ultrashort and intense laser pulses as well ashigh power synchrotron radiation sources and x-ray free electronlasers have promoted fast developments in nonlinear optics andx-ray spectroscopy.The new experimental achievements and the appearance of varieties of novelnonlinear phenomena call for further development of theories. The objective of this thesis is to develop and apply thetheories to explain existing experimental data and to suggest new experiments. The first part of the thesis is devoted to nonlinear propagation of optical pulses. It is shown that the vibrational levels can be selectively populated by varying the duration, shape and intensity of the pump pulse. We obtained a strict analytical solution for the resonant two-photon interaction in a multilevel system beyond rotating wave approximation. Simulations show that the polarization anisotropy of the two-photon excitation affects strongly the anisotropy of photobleaching.The two-photon area theorem is reformulated with taking into account the dynamical Stark shift and the contribution from the permanent dipole moments. In general the dynamical Stark shift does not allow complete population of the excited state, but it can be compensated by detunings in atoms. A dynamical theory of the sequential two-photon absorption of  microsecond pulses  is developed to explore the role of transverse inhomogeneity of the light beam on optical limiting properties.  The propagation of ultrashort laser pulses in nondipolar and dipolar media is investigated with special attention to the generation of superfluorescence and supercontinuum and the formation of attosecond pulses. The second part of the thesis addresses the interaction of molecules with x-ray radiation.  We explore here the role of nuclear dynamics in resonant Auger scattering. Multimode simulations of the Auger spectra of ethylene molecule explain the main spectral features of the experimental spectra and show that the spectral profiles are formed mainly due to six vibrational modes. We predict the Doppler splitting of the atomic peak in resonant Auger scattering from SF6 molecule for circularly polarized x-rays. This effect is confirmed by the recent experiment. A new scheme of x-ray pump-probe spectroscopy, namely, resonant inelastic x-ray scattering accompanied by core-hole hopping induced by strong laser fields is suggested. The laser-induced promotion of core holes opens the symmetry forbidden scattering channels and gives rise to new spectral lines in the x-ray scattering spectrum. The strength of the symmetry forbidden lines becomes strong when  the time of Rabi flopping is shorter than the lifetime of the core-excited state. We study the role of propagation of femtosecond x-ray free-electron pulses on the Auger process. Simulations show  that there exists a strong competition between Auger decay and stimulated emission. The Auger yield and Auger branching ratio are strongly suppressed in the course of pulse propagation. / QC 20100729

Fluorescence microscopy allows for spatial and temporal resolution of systems which are inherently fluorescent or which can be selectively labeled with fluorescent molecules. Temporal resolution is crucial for imaging real time processes in living samples. A common problem in fluorescence microscopy of biological samples is autofluorescence, fluorescence inherent to the system, which interferes with detection of fluorescence of interest by decreasing the signal to noise ratio. Two current methods for improved imaging against autofluorescence are two-photon excitation and total internal reflection microscopy. Two-photon excitation occurs when two longer wavelength photons are absorbed quasi-simultaneously by a single fluorophore. For this to take place there must be a photon density on the order of 1030 photons/(cm2)(s), which is achieved through use of a femtosecond pulsed laser and a high magnification microscope objective. Two-photon excitation then only occurs at the focal spot, significantly reducing the focal volume and therefore background autofluorescence. The second method, total internal reflection, is based on evanescent wave excitation, which decreases exponentially in intensity away from the imaging surface. This allows for excitation of a thin (~200 nm) slice of a sample. Since only a narrow region of interest is excited, an optical slice can be imaged, decreasing excitation of out-of-focus autofluorescence, and increasing the signal to noise ratio. By coupling total internal reflection with two-photon excitation, an entire cell can be imaged while still maintaining the use of lower energy photons to irradiate the sample and achieve two-photon excitation along the length traveled by the evanescent wave. This system allows for more sensitive detection of fluorescence of interest from biological systems as a result of a significant decrease in excitation volume and therefore a decrease in autofluorescence signal. In the two-photon total internal reflection microscopy setup detailed in this work, an excitation area of 20 μm by 30 μm is achieved, and used to image FITC-stained actin filaments in BS-C-1 cells

Thesis (Ph. D.)--Physics, Georgia Institute of Technology, 2008. / Committee Chair: Uzer, Turgay; Committee Member: Aral, Mustafa; Committee Member: Flannery, Raymond; Committee Member: Raman, Chandra; Committee Member: Schatz, Michael.

The general goal of this dissertation is to provide a comprehensive description of the limitations of established theories on bound electronic nonlinearities in direct-gap semiconductors by performing various experiments on wide and narrow bandgap semiconductors along with developing theoretical models. Nondegenerate two-photon absorption (2PA) is studied in several semiconductors showing orders of magnitude enhancement over the degenerate counterpart. In addition, three-photon absorption (3PA) is studied in ZnSe and other semiconductors and a new theory using a Kane 4-band model is developed which fits new data well. Finally, the narrow gap semiconductor InSb is studied with regard to multiphoton absorption, free-carrier nonlinearities and decay mechanisms. The non-degenerate two-photon absorption was investigated in several direct-gap semiconductors with picosecond and femtosecond pulses. Large enhancements in 2PA were demonstrated when employing highly non-degenerate photon pairs and the results were shown to be consistent to a simple 2-parabolic band theory based on a "dressed" state approach. The nonlinear refractive index induced in such configurations was also calculated and possible implications of such extreme behavior are discussed. A large number of measurements of 3PA were taken at multiple wavelengths and in several semiconductors. The subsequent analysis has shown that simple 2-band model calculations (based on either perturbative or tunneling approaches) do not adequately describe the experimental trends. A more comprehensive model, based on Kane’s 4-band theory was developed and we calculate three-photon spectra for zincblende structures within the perturbative iv framework. We have confirmed the results of our calculations performing a series of Z-scans in semiconductors ZnSe and ZnS, yielding complete experimental three-photon spectra. A systematic approach based on using a large variety of pulse durations was needed to quantify the wealth of nonlinear optical processes in InSb, accessible in the mid-infrared range. Femtosecond pulses provided a lower limit to measurements of the instantaneous effects (absorptive and refractive), while picosecond pulses allowed further characterization of the freecarrier effects, including population dynamics in the high density regime (Auger effects). The model developed permitted us to verify the temperature dependence of free-carrier absorption recently predicted, and to successfully model optical limiting data with longer, nanosecond pulses.