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The dynamics of ultrashort pulse generation and amplification in dye lasers is studied in this dissertation. In particular, we have developed general semiclassical models for ultrashort pulse dye laser amplifiers and oscillators. These models start from Maxwell’s equation for the electric field and density matrix equations for the active laser medium. A finite coherence time or phase memory time of the molecular wave functions, a finite vibrational relaxation time for the lower electronic state of the dye laser transition, an isotropic molecular orientational distribution, and an arbitrary pump polarization are all taken into account. Based on these models, specific topics that are discussed herein include pump polarization effects, timing and detuning studies in synchronously pumped mode-locked dye lasers, and amplification of ultrashort pulses in dye laser amplifiers. Properties such as pulse width, pulse shape, pulse intensity, pulse stability, pulse amplification efficiency, etc., are studied in detail.

In this thesis the interaction of ultrashort laser pulses with metal nanostructures is investigated via two different phenomena: coherent acoustic oscillations of nanoparticles and generation of THz pulses on metal surfaces. Both of these effects rely on the collective oscillations of free conduction electrons in metal surfaces, plasmons. The field of plasmonics gained a great interest in the last twenty years due to the unique properties of these surface modes. It is the effects of the resonant response of plasmonic structures to incident electromagnetic wave, in particular, in visible and infrared bands and the concentration of the electromagnetic field in small subwavelength regions with significant enhancement of the incident field that make plasmonics so attractive for various applications, such as biochemical sensing, enhanced fluorescence, surface-enhanced Raman scattering, and second harmonic generation, amongst others. Investigation of the coherent particle vibrations is performed using the pump-probe technique which allows measurement of the transient transmission signals. The expansion and subsequent contraction of the nanoparticle following the ultrashort laser pulse excitation lead to a shift of the plasmon band which can be traced by transient spectroscopy. We have investigated the effect of the particle thickness on the frequency of the fundamental vibrational mode. In addition, we measured the vibrational particle response during the particle shape deformation, both symmetrical and asymmetrical. Exploration of the THz generation phenomena on plasmonic structures was performed using THz time-domain spectroscopy, the method which allows tracing of the generated THz field in the time-domain. We were able for the first time to measure the THz pulses generated from arrays of metal nanoparticles. Our observations verify the role of the particle plasmon mode in the generation of THz pulses. In addition, by exploring the dependence of the THz emission on the femtosecond pulse intensity we showed a high nonlinearity in the THz generation mechanism. The experimental results were assessed in the context of a recently proposed model where the THz radiation is generated via the acceleration of the ejected electrons by ponderomotive forces. To reveal another proposed mechanism of the THz generation from plasmonic structures, namely optical rectification, we investigated the THz generation and electron emission from the arrays of nanoparticles and nanoholes. Our results suggest that both mechanisms may contribute to generation of THz pulses from the same sample under different illumination conditions. In addition to periodic arrays of nanoparticles and nanoholes, THz generation from random metal-dielectric films was investigated. The microstructuring of such films allowed selective THz frequency generation which was explained by a model of dipole THz emitters. In addition, the effects of low temperature and pressure on the THz generation efficiency were investigated.

In this thesis we ran a series of 2D simulations of femtosecond laser pulses filamenting in air using the FDTD method, a saturable Lorentz oscillator model of air [1], and two separate models of plasma: a Drude model where the plasma density is static in space, and a particle-in-cell model where plasma is free to migrate throughout the simulation space. By comparing matched pairs of simulations, which varied in pulse size, duration, and intensity, we can gauge the impact plasma dynamics has upon the evolution of a filamenting laser pulse. From these tests we determine that, while there are some visible differences between dynamic and static plasmas, plasma dynamics do not significantly alter the evolution of the pulse.

The concern of this dissertation is the understanding and improvement of a class of lasers that is responsible for some of the shortest optical pulses available today. In particular, we seek ways to produce from synchronously pumped mode-locked dye laser systems, shorter pulses of higher intensity with improved pulse-to-pulse consistency. Specific topics.that are discussed herein include the study of the role of the pump pulse in synchronously pumped mode-locked lasers, the study of the pulse shaping and shortening due to an intracavity saturable absorber, and the study of a fundamental pulse train instability associated with these lasers.

Revestimentos superficiais são aplicados à muitas ferramentas de usinagem na indústria metalúrgica com o intuito de melhorar a eficiência de corte e aumentar sua vida útil. Neste trabalho foram realizados testes para remoção do recobrimento de nitreto de titânio alumínio (TiAlN) em pastilhas de carboneto de tungstênio (WC-Co), utilizando um feixe laser de pulsos ultracurtos. Após a determinação dos limiares de dano do filme e do substrato foram ablacionados na superfície do recobrimento, traços utilizando duas condições de ablação. Inicialmente operou-se no regime de baixa fluência do filme, e posteriormente no regime de baixa fluência do substrato, muito abaixo do limiar do filme, aplicando-se alta sobreposição de pulsos. Um sistema de espectroscopia de emissão atômica induzida por laser (LIBS) foi montado para monitoramento dos materiais presentes no plasma gerado pelo laser, porém o sistema não apresentou sensibilidade suficiente para leitura da baixa intensidade do plasma proveniente do processo e não foi utilizado. Após a análise dos traços por microscopia eletrônica, perfilometria óptica e espectroscopia por fluorescência de Raios-X, não foi possível determinar um processo seguro para realizar a remoção seletiva do filme em questão, porém, devido aos dados obtidos e observações dos resultados em alguns traços, novas possibilidades foram levantadas, abrindo a discussão para a realização de trabalhos futuros. / Surface coatings are applied to many cutting tools in the metallurgical industry in order to improve cutting efficiency and extend its useful life. In this work, tests were performed to remove the coating of titanium aluminum nitride (TiAlN) on tungsten carbide (WC-Co) pellets, using an ultrashort laser pulses beam. After determination of the damage thresholds of the film and the substrate, were ablated on the surface of the coating lines using two ablation conditions, it was initially operated on the low fluence regime for the film, and later on the low fluence regime of the substrate, far below the threshold of the film, applying high overlapping pulses. A laser induced breakdown spectroscopy (LIBS) system was set up to monitor the materials present in the plasma generated by the laser, but the system did not present sufficient sensitivity to read the low intensity of the plasma generated in the process and was not used. After the analysis of the traces by electron microscopy, optical profilometer and X-ray fluorescence spectroscopy, it was not possible to determine a safe process to carry out the selective removal of the film in question, however, due to the data obtained and observations of the results in some traces, new possibilities were raised, opening the discussion for future work.

Revestimentos superficiais são aplicados à muitas ferramentas de usinagem na indústria metalúrgica com o intuito de melhorar a eficiência de corte e aumentar sua vida útil. Neste trabalho foram realizados testes para remoção do recobrimento de nitreto de titânio alumínio (TiAlN) em pastilhas de carboneto de tungstênio (WC-Co), utilizando um feixe laser de pulsos ultracurtos. Após a determinação dos limiares de dano do filme e do substrato foram ablacionados na superfície do recobrimento, traços utilizando duas condições de ablação. Inicialmente operou-se no regime de baixa fluência do filme, e posteriormente no regime de baixa fluência do substrato, muito abaixo do limiar do filme, aplicando-se alta sobreposição de pulsos. Um sistema de espectroscopia de emissão atômica induzida por laser (LIBS) foi montado para monitoramento dos materiais presentes no plasma gerado pelo laser, porém o sistema não apresentou sensibilidade suficiente para leitura da baixa intensidade do plasma proveniente do processo e não foi utilizado. Após a análise dos traços por microscopia eletrônica, perfilometria óptica e espectroscopia por fluorescência de Raios-X, não foi possível determinar um processo seguro para realizar a remoção seletiva do filme em questão, porém, devido aos dados obtidos e observações dos resultados em alguns traços, novas possibilidades foram levantadas, abrindo a discussão para a realização de trabalhos futuros. / Surface coatings are applied to many cutting tools in the metallurgical industry in order to improve cutting efficiency and extend its useful life. In this work, tests were performed to remove the coating of titanium aluminum nitride (TiAlN) on tungsten carbide (WC-Co) pellets, using an ultrashort laser pulses beam. After determination of the damage thresholds of the film and the substrate, were ablated on the surface of the coating lines using two ablation conditions, it was initially operated on the low fluence regime for the film, and later on the low fluence regime of the substrate, far below the threshold of the film, applying high overlapping pulses. A laser induced breakdown spectroscopy (LIBS) system was set up to monitor the materials present in the plasma generated by the laser, but the system did not present sufficient sensitivity to read the low intensity of the plasma generated in the process and was not used. After the analysis of the traces by electron microscopy, optical profilometer and X-ray fluorescence spectroscopy, it was not possible to determine a safe process to carry out the selective removal of the film in question, however, due to the data obtained and observations of the results in some traces, new possibilities were raised, opening the discussion for future work.

Chirped Bragg gratings (CBGs) recorded in photo-thermo-refractive (PTR) glass provide a very efficient and robust way to stretch and compress ultra-short laser pulses. These gratings offer the ability to stretch pulses from hundreds of femtoseconds, to the order of 1 ns and then recompress them. However, in order to achieve pulse stretching of this magnitude, 100 mm thick CBGs are needed. Using these CBGs to both stretch, and re-compress the pulse thus requires propagation through 200 mm of optical glass. This therefore demands perfect control of the glass homogeneity, as well as the holographic recording process of the CBG. In this thesis, we present a study of the CBG parameters that lead to distortions in the quality of diffracted beams. We first present the challenges associated with measuring the quality of these beams and we show that such measurements are not easily achieved using commercial systems that rely on the ISO standard M2 method. Thus, we introduce a new metric of beam quality, which we have coined S2 , that is a combination of both the M2 and power in the bucket metrics. Subsequently, we investigate the influence of the CBG parameters on the quality of diffracted beams. In particular, we examine the impact of small optical heterogeneities known as striae, as well as the impact of the optically and thermally induced distortions in the grating. We then use this data to improve the fabrication and characterization of 100 mm long CBGs. Finally, we characterize the performance of CBGs recorded in PTR for stretching and compression of femtosecond pulses using a custom autocorrelation system. We present data on high quality 100 mm long CBGs and an analysis on the correlation between beam quality and the final pulse duration after stretching and re-compressing the pulse.

In this thesis, advanced spectroscopy methods are discussed and applied to gain understanding of the physical properties of organic conjugated molecules, II-VI thin film semiconductors, and vertical cavity surface emitting lasers (VCSEL). Experiments include single photon and two-photon excitation with lasers, with subsequent measurements of the absorption and photoluminescence, as well as photocurrent measurements using tungsten and xenon lamps, measuring the direct current and the alternating current of the devices. The materials are investigated in dissolved form (conjugated polymers), thin films (polymers, II-VI semiconductors), and complex layer structures (hybrid device, VCSEL). The experiments are analyzed and interpreted by newly developed or applied theories for two-photon saturation processes in semiconductors, bandgap shrinkage due to optically induced electron hole pairs, and the principle of detailed balance to describe the photoluminescence in thin film cadmium sulfide. / Ph. D.