Neste trabalho investigamos as propriedades térmicas (difusividade, condutividade, variação do caminho óptico com a temperatura, etc) e processos de perdas devido a interações entre íons em materiais lasers vítreos e cristalinos. Desde que a eficiência quântica de fluorescência, , está diretamente relacionada com esses mecanismos que levam a supressão da luminescência, os estudos foram realizados principalmente observando os efeitos desses agentes sobre . Espectros de lente térmica (LT) foram usados para determinar , eficiência de transferência de energia matriz-íon, e para analisar efeitos de sítios de defeitos sobre . Um novo método usando a técnica de LT foi proposto para determinar e o coeficiente de temperatura do caminho óptico. Com esta nova abordagem analisamos em materiais vítreos os mecanismos de supressão da luminescência em função da concentração de íons de Nd. Também a usamos para estudar efeitos de radicais de OH e outras impurezas em matrizes vítreas de fosfato dopadas com Yb3+. Processos de conversão ascendente Auger, os quais são importantes em sistemas lasers de alta potência, foram investigados em vidros e cristais dopados com Nd3+. Nos vidros o estudo foi realizado em função da concentração de íons dopantes. Neste estudo a técnica de LT mostrou ser muito sensível, apresentando resultados com erros bem menores que os existentes na literatura. Seguindo o estudo de perdas, investigamos distorção óptica induzida pela luz em função da temperatura, potência de excitação e polarização no cristal ferroelétrico SBN. Usando a técnica de LT, investigamos as propriedades térmicas através da transição de fase ferroelétrica-paraelétrica em cristais de SBN. Complementando, esta tese contribui significativamente para a caracterização de materiais laser, considerando que vários dos mecanismos de perdas estudados propriamente devem ser levados em conta em projetos de laser. Este trabalho também apresenta a técnica de lente térmica como uma ferramenta valiosa para tal estudo. / In this work we investigate the thermal properties (diffusivity, conductivity, temperature coefficient of the optical path length change, etc) and loss processes owing to ion-ion interactions in laser glassy and crystalline materials. Since the fluorescence quantum efficiency, , is directly related to these mechanisms that lead to luminescence quenching, the studies were performed mainly observing the effects of these processes on . Thermal lens (TL) spectra were used to determine , energy transfer efficiency between matrix-ion, and to analyze effects of \"dead site\" on . A new method based on the TL technique was proposed to determine q and the temperature coefficient of the optical path length change. This new approach was used to investigate concentration quenching mechanisms in glassy materials. It was also used to study effects of OH radicals and other impurities in Yb3+ doped phosphate glasses. Upconversion Auger processes, which are very important for high power laser systems, were investigated in Nd3+ -doped glasses and crystals. In glasses the study was performed as a function of doping ions. In this study the TL showed to be very sensitive, presenting results with uncertainties much smaller than previous literatures. Following the study of losses, we investigate light induced optical distortion as a function of temperature, excitation power, and polarization in SNB ferroelectric crystal. Using the TL technique, the thermal properties through the phase transition ferroelectric-paraelectric in SBN crystals were investigated. In addition, this thesis significantly contributes for characterization of laser materials with potential applications, considering that severa1 of the loss mechanisms studied here must be considered in laser design. This work also presents the TL technique as a valuable to01 for the present study.

Neste trabalho investigamos as propriedades térmicas (difusividade, condutividade, variação do caminho óptico com a temperatura, etc) e processos de perdas devido a interações entre íons em materiais lasers vítreos e cristalinos. Desde que a eficiência quântica de fluorescência, , está diretamente relacionada com esses mecanismos que levam a supressão da luminescência, os estudos foram realizados principalmente observando os efeitos desses agentes sobre . Espectros de lente térmica (LT) foram usados para determinar , eficiência de transferência de energia matriz-íon, e para analisar efeitos de sítios de defeitos sobre . Um novo método usando a técnica de LT foi proposto para determinar e o coeficiente de temperatura do caminho óptico. Com esta nova abordagem analisamos em materiais vítreos os mecanismos de supressão da luminescência em função da concentração de íons de Nd. Também a usamos para estudar efeitos de radicais de OH e outras impurezas em matrizes vítreas de fosfato dopadas com Yb3+. Processos de conversão ascendente Auger, os quais são importantes em sistemas lasers de alta potência, foram investigados em vidros e cristais dopados com Nd3+. Nos vidros o estudo foi realizado em função da concentração de íons dopantes. Neste estudo a técnica de LT mostrou ser muito sensível, apresentando resultados com erros bem menores que os existentes na literatura. Seguindo o estudo de perdas, investigamos distorção óptica induzida pela luz em função da temperatura, potência de excitação e polarização no cristal ferroelétrico SBN. Usando a técnica de LT, investigamos as propriedades térmicas através da transição de fase ferroelétrica-paraelétrica em cristais de SBN. Complementando, esta tese contribui significativamente para a caracterização de materiais laser, considerando que vários dos mecanismos de perdas estudados propriamente devem ser levados em conta em projetos de laser. Este trabalho também apresenta a técnica de lente térmica como uma ferramenta valiosa para tal estudo. / In this work we investigate the thermal properties (diffusivity, conductivity, temperature coefficient of the optical path length change, etc) and loss processes owing to ion-ion interactions in laser glassy and crystalline materials. Since the fluorescence quantum efficiency, , is directly related to these mechanisms that lead to luminescence quenching, the studies were performed mainly observing the effects of these processes on . Thermal lens (TL) spectra were used to determine , energy transfer efficiency between matrix-ion, and to analyze effects of \"dead site\" on . A new method based on the TL technique was proposed to determine q and the temperature coefficient of the optical path length change. This new approach was used to investigate concentration quenching mechanisms in glassy materials. It was also used to study effects of OH radicals and other impurities in Yb3+ doped phosphate glasses. Upconversion Auger processes, which are very important for high power laser systems, were investigated in Nd3+ -doped glasses and crystals. In glasses the study was performed as a function of doping ions. In this study the TL showed to be very sensitive, presenting results with uncertainties much smaller than previous literatures. Following the study of losses, we investigate light induced optical distortion as a function of temperature, excitation power, and polarization in SNB ferroelectric crystal. Using the TL technique, the thermal properties through the phase transition ferroelectric-paraelectric in SBN crystals were investigated. In addition, this thesis significantly contributes for characterization of laser materials with potential applications, considering that severa1 of the loss mechanisms studied here must be considered in laser design. This work also presents the TL technique as a valuable to01 for the present study.

This thesis reports on the development of glass-based femtosecond laser sources around 2 µm wavelength. In order to be able to produce 2 µm radiation the dopants used were trivalent Thulium (Tm³⁺) and trivalent Holmium (Ho³⁺) that could be optically pumped with Ti:Sapphire radiation at 0.8 µm and semiconductor disk lasers (SDL) at 1.2 µm. The samples were produced at Leeds University and polished in-house in bulk form and deployed in free space laser cavities. Tellurite compounds doped with Tm³⁺ produced stable continuous wave 1.94 µm radiation when pumped at 800 nm with a maximum efficiency of 28.4% with respect to the absorbed power and maximum output power around 120 mW when pumped using a Ti:Sapphire operating around 0.8 µm. The radiation was broadly tunable across 130 nm. Tm³⁺-Ho³⁺ doubly doped tellurite samples lased around 2.02 µm with maximum efficiency of 25.9% and with P[subscript(OUT)]=75 mW and a smooth tunability of 125 nm. The fluorogermanate glass doped with Tm³⁺ gave an absorbed to output power efficiency of 50%. The maximum continuous wave output powers obtained were around 190 mW and limited by the available pump power at 0.8 µm. These results together with a very low threshold of 60 mW of incident power were comparable to the crystalline counterparts to this gain medium. The Tm3+ tellurite and the Tm³⁺-Ho³⁺ tellurite compounds were also pumped by an SDL operating at 1215 nm to obtain an indication of the viability of such a pump scheme. The results were a maximum internal slope efficiency of 22.4% with a highest output power of 60 mW. The comparison demonstrated that 1.2 µm pumping was competitive with using 0.8 µm wavelength. The use of semiconductor saturable absorbing mirror (SESAM) technology was used for the modelocking of these lasers. The SESAM was produced in Canada and implanted with As⁺ ions in order to reduce the relaxation time. Trains of transform-limited laser pulses at 222 MHz as short as 410 fs centred at 1.99 µm were produced for the first time with a bulk Tm³⁺:Fluorogermanate glass. The maximum average output power obtained was of 84 mW. The same SESAM deployed on the Tm³⁺-Ho³⁺ Tellurite compounds gave trains of transform-limited pulses as short as 630 fs at 2.01 µm with a repetition rate of 143 MHz and a maximum averaged output power of 43 mW. The regime of propagation obtained was soliton-like and the modelocking was self-starting. The results obtained with bulk glass were very promising and open interesting research pathways within the realm of amorphous bulk gain media.

This thesis describes a number of studies on organic semiconductors focused around using them as gain media for lasers. The photophysical properties of organic semiconductors are studied using a wide range of experimental techniques, allowing the evaluation of new materials and novel excitation schemes for use in organic semiconductor lasers. Polyfluorene is a well-established conjugated polymer laser gain medium and in this thesis its excellent lasing properties are combined with its two photon absorption properties to demonstrate a tunable two-photon pumped solid-state laser based on a commercially available organic semiconductor. A family of bisfluorene dendrimers was studied using a number of photophysical techniques to evaluate their potential as laser materials. Distributed feedback lasers based on one of the dendrimers are demonstrated with lasing thresholds comparable to polyfluorene. The same materials were found to have enhanced two-photon absorption properties in comparison to polyfluorene, leading to the fabrication of tunable two-photon pumped dendrimer lasers. A member of a novel family of star-shaped oligofluorene truxenes was evaluated as a laser gain material and the distributed feedback lasers made from them show some of the lowest lasing thresholds reported for organic semiconductors, partly as a consequence of exceptionally low waveguide losses in comparison to other single-material thin films. Finally, an organic laser dye is blended with a conjugated polymer, where the dye molecules harvest the excitation light of a GaN laser diode and transfer its energy to the polymer molecules. This is the first time such a scheme is used in an organic laser and in combination with a novel surface-emitting distributed Bragg reflector resonator allows the demonstration of a diode-pumped organic laser, a significant step towards simplifying organic lasers.

In this work, we have investigated the thermal properties (diffusivity (D), conductivity (K), temperature coefficient of the optical path length change (ds/dT), etc) and loss processes owing to the ion-ion interactions, in Nd3+ doped laser materials, specifically YAG ceramic and CGGG crystal. Since the fluorescence quantum efficiency, , is directly related to these mechanisms that lead to luminescence quenching, the studies were carried out mainly observing the effects of these processes on . To this goal we used mainly the thermal lens technique and conventional spectroscopy. In Nd:YAG ceramic, we have investigated the losses due to down-conversion or, as they are well known, concentration quenching that are basically cross relaxation (CR) and energy migration (EM). From these results, it was concluded that the main source of luminescence quenching is CR and that the small ds/dT value together with the high optimum concentration put this material as candidate for several applications. In Nd:CGGG crystal, we have studied the loss processes owing to upconversion or, as is better known, upconversion Auger (UA) or energy transfer upconversion, which are important in laser systems of high. / Fundação de Amparo a Pesquisa do Estado de Alagoas / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / Neste trabalho investigamos as propriedades térmicas (difusividade (D), condutividade (K), variação do caminho óptico com a temperatura (ds/dT), etc) e processos de perdas devido a interações entre íons, em materiais lasers dopados com Nd3+, especificamente cerâmica de YAG e cristal CGGG. Desde que a eficiência quântica de fluorescência, , está diretamente relacionada com esses mecanismos que levam a supressão da luminescência, os estudos foram realizados principalmente observando os efeitos desses agentes sobre . Para esse propósito, usamos principalmente a técnica de lente térmica e espectroscopia convencional. Na cerâmica de Nd:YAG investigamos as perdas por down-conversion ou, como é melhor conhecidas, quenching de concentração que são basicamente relaxação cruzada (RC) e migração de energia (ME). Nesses resultados concluímos que a principal fonte de supressão da luminescência é RC e que o valor de ds/dT baixo juntamente com a concentração ótima alta apresentam esse material com boas perspectivas de aplicações. No cristal Nd:CGGG estudamos os processos de perdas por upconversion ou, como é melhor conhecido, conversão ascendente Auger (CAA) ou conversão ascendente por transferência de energia, os quais são importantes em sistemas lasers de alta potência e/ou altas concentrações de íons dopantes. Com a presença dos processos de CAA é adicionado mais um canal de decaimento não radiativo. E como resultado foi observado uma diminuição de η e consequentemente um aumento da carga térmica (φ). O conhecimento dos processos investigados nesta dissertação é de importância fundamental para a engenharia e caracterização de matérias lasers.

Lasers find a wide range of applications in many areas including photo-biology, photo-chemistry, materials processing, imaging and telecommunications. However, the practical use of such sources is often limited by the bulky nature of existing systems. By fabricating channel waveguides in solid-state laser-gain materials more compact laser systems can be designed and fabricated, providing user-friendly sources. Other advantages inherent in the use of waveguide gain media include the maintenance of high intensities over extended interaction lengths, reducing laser thresholds. This thesis presents the development of Yb:tungstate lasers operating around 1μm in waveguide geometries. An Yb:KY(WO₄)₂ planar waveguide laser grown by liquid phase epitaxy is demonstrated with output powers up to 190 mW and 76 % slope efficiency. This is similar to the performance from bulk lasers but in a very compact design. Excellent thresholds of only 40 mW absorbed pump power are realised. The propagation loss is found to be less than 0.1 dBcm⁻¹ and Q-switched operation is also demonstrated. Channel waveguides are fabricated in Yb:KGd(WO₄)₂ and Yb:KY(WO₄)₂ using ultrafast laser inscription. Several of these waveguides lase in compact monolithic cavities. A maximum output power of 18.6 mW is observed, with a propagation loss of ~2 dBcm⁻¹. By using a variety of writing conditions the optimum writing pulse energy is identified. Micro-spectroscopy experiments are performed to enable a fuller understanding of the induced crystal modification. Observations include frequency shifts of Raman lines which are attributed to densification of WO₂W bonds in the crystal. Yb:tungstate lasers can generate ultrashort pulses and some preliminary work is done to investigate the use of quantum dot devices as saturable absorbers. These are shown to have reduced saturation fluence compared to quantum well devices, making them particularly suitable for future integration with Yb:tungstate waveguides for the creation of ultrafast, compact and high repetition rate lasers.