Thesis--Wisconsin. / Vita. Includes bibliographical references.

Thesis (Ph. D. in materials science)--Washington State University. / Includes bibliographical references.

No description available.

Nesta trabalho estudamos o efeito de refração não linear em cristais fluoretos dopados com Cr+3 e polímeros. Tais cristais fluoretos têm recebido bastante atenção dos pesquisadores por apresentarem um espectro de emissão de banda larga e ação laser sintonizável na região de aproximadamente 780-1010 nm. Aplicando a técnica de lente Térmica (LT), realizamos um estudo quantitativo do comportamento da eficiência quântica de emissão, na presença dos processos de supressão térmica da fluorescência e conversão ascendente. Apresentamos um novo método de aplicação da técnica de LT, que possibilita a determinação da eficiência quântica em função do parâmetro de saturação S (S= IM/Is, em que IM é a intensidade média incidente no material e Is a intensidade de saturação). A partir desses resultados é possível determinar o parâmetro de conversão ascendente Auger (γ), desde que se conheça a população total do Cr+3 ( N0) e o tempo de vida de emissão τ(τ-1=τR-1+τNR-1) do material investigado. Este método é apresentado para LiSAF dopados com 1% e 7% de Cr+3 , e LiSGaF 4.7% de dopagem de Cr+3, excitados em regime cw sob 15°C. No caso dos polímeros, estudamos a caracterização das propriedades não lineares (eletrônica e térmica) das amostras de polianilina (PANI) dopadas e não-dopadas com H2SO4 na forma plastificada e dissolvida em dimetil sulfóxido (DMSO). Utilizamos para isso as técnicas de LT (cw) e Z-scan (cw e pulso de 70 ps). As medidas foram realizadas em função da concentração de PANI e temperatura. Utilizando um laser de Nd:YAG com um trem de pulsos, realizamos um estudo dinâmico da não linearidade em função da concentração da PANI. Dessa forma pudemos discriminar o efeito eletrônico do efeito térmico, determinando o índice de refração não linear (n2f) um índice térmico (n2cth) que está relacionado ao parâmetro térmico dn/dT (variação do coeficiente óptico com a temperatura). / In this work we studied the effect of nonlinear refraction in Cr+3 doped fluoride host crystals and polymers. The fluoride crystals have been attractive due a broad emission bandwidth and a tunable solid-state lasing in the range of approximately 780-1010 nm. Applying the Thermal Lens (TL) technique, we accomplished a quantitative study of the behavior of the quantum efficiency, in the presence of the processes of the fluorescence thermal quenching and upconversion processes. We introduced a new method of application of the TL technique, which makes possible the determination of the quantum efficiency as a function of the saturation parameter S (S= IM/Is, where IM is the medium intensity in the material and Is, the saturation intensity). Based on those results it is possible to determine the Auger upconversion parameter (γ), it one knows the total population of Cr+3 (N0) and the emission lifetime τ(τ-1=τR-1+τNR-1) of the investigated material. This method is presented for 1% and 7% Cr+3 doped LiSAF, and 4.7% of Cr+3 doped LiSGaF, upon excitation in the cw regime at 15°C. In the case of the polymers, we studied the nonlinear properties (electronics and thermal nonlinearities) of the polyaniline samples (PANI) doped and nondoped with H2SO4 in the film form and dissolved in dimethylsulfoxide. We used the LT (cw) and Z-scan (cw and pulse of 70 ps) techniques. The measurements were accomplished as a function of the concentration of PANI and temperature. Using a laser of Nd:YAG with pulse trains, we accomplished the dynamic behavior of the optical nonlinearity as a function of the PANI concentration. By this method we were able to discriminate between electronic and thermal lensing nonlinearities, and allows the determination of the nonlinear refractive index (n2f) and thermal index (n2cth) that is related to the thermal parameter dn/dT (temperature coefficient of refractive index).

Nesta trabalho estudamos o efeito de refração não linear em cristais fluoretos dopados com Cr+3 e polímeros. Tais cristais fluoretos têm recebido bastante atenção dos pesquisadores por apresentarem um espectro de emissão de banda larga e ação laser sintonizável na região de aproximadamente 780-1010 nm. Aplicando a técnica de lente Térmica (LT), realizamos um estudo quantitativo do comportamento da eficiência quântica de emissão, na presença dos processos de supressão térmica da fluorescência e conversão ascendente. Apresentamos um novo método de aplicação da técnica de LT, que possibilita a determinação da eficiência quântica em função do parâmetro de saturação S (S= IM/Is, em que IM é a intensidade média incidente no material e Is a intensidade de saturação). A partir desses resultados é possível determinar o parâmetro de conversão ascendente Auger (γ), desde que se conheça a população total do Cr+3 ( N0) e o tempo de vida de emissão τ(τ-1=τR-1+τNR-1) do material investigado. Este método é apresentado para LiSAF dopados com 1% e 7% de Cr+3 , e LiSGaF 4.7% de dopagem de Cr+3, excitados em regime cw sob 15°C. No caso dos polímeros, estudamos a caracterização das propriedades não lineares (eletrônica e térmica) das amostras de polianilina (PANI) dopadas e não-dopadas com H2SO4 na forma plastificada e dissolvida em dimetil sulfóxido (DMSO). Utilizamos para isso as técnicas de LT (cw) e Z-scan (cw e pulso de 70 ps). As medidas foram realizadas em função da concentração de PANI e temperatura. Utilizando um laser de Nd:YAG com um trem de pulsos, realizamos um estudo dinâmico da não linearidade em função da concentração da PANI. Dessa forma pudemos discriminar o efeito eletrônico do efeito térmico, determinando o índice de refração não linear (n2f) um índice térmico (n2cth) que está relacionado ao parâmetro térmico dn/dT (variação do coeficiente óptico com a temperatura). / In this work we studied the effect of nonlinear refraction in Cr+3 doped fluoride host crystals and polymers. The fluoride crystals have been attractive due a broad emission bandwidth and a tunable solid-state lasing in the range of approximately 780-1010 nm. Applying the Thermal Lens (TL) technique, we accomplished a quantitative study of the behavior of the quantum efficiency, in the presence of the processes of the fluorescence thermal quenching and upconversion processes. We introduced a new method of application of the TL technique, which makes possible the determination of the quantum efficiency as a function of the saturation parameter S (S= IM/Is, where IM is the medium intensity in the material and Is, the saturation intensity). Based on those results it is possible to determine the Auger upconversion parameter (γ), it one knows the total population of Cr+3 (N0) and the emission lifetime τ(τ-1=τR-1+τNR-1) of the investigated material. This method is presented for 1% and 7% Cr+3 doped LiSAF, and 4.7% of Cr+3 doped LiSGaF, upon excitation in the cw regime at 15°C. In the case of the polymers, we studied the nonlinear properties (electronics and thermal nonlinearities) of the polyaniline samples (PANI) doped and nondoped with H2SO4 in the film form and dissolved in dimethylsulfoxide. We used the LT (cw) and Z-scan (cw and pulse of 70 ps) techniques. The measurements were accomplished as a function of the concentration of PANI and temperature. Using a laser of Nd:YAG with pulse trains, we accomplished the dynamic behavior of the optical nonlinearity as a function of the PANI concentration. By this method we were able to discriminate between electronic and thermal lensing nonlinearities, and allows the determination of the nonlinear refractive index (n2f) and thermal index (n2cth) that is related to the thermal parameter dn/dT (temperature coefficient of refractive index).

The spectroscopy of wide-bandgap fluoride materials doped with divalent ytterbium is presented. The structure of impurity-trapped excitons is explored, vacuum ultraviolet excitation is used to investigate the transfer processes between excitations, and the effect of confinement on self-trapped excitons is studied. The excited-state structure of impurity-trapped excitons is measured in the multisite system NaMgF₃:Yb²⁺. A two-colour ultraviolet-infrared pulsed photoluminescence enhancement technique is employed to probe the interlevel transitions and dynamics of impurity-trapped excitons in doped insulating phosphor materials. NaMgF₃:Yb²⁺ exhibits emission from two charge-compensation centres with peaks at 22 300 cm⁻¹ (448 nm) and 24 000 cm⁻¹ (417 nm). The observed photoluminescence enhancement is caused by a combination of intra-excitonic excitation and electron trap liberation. The electron traps are inferred to have a depth of approximately 800 cm⁻¹. Time-resolved VUV spectroscopic studies of emission and excitation spectra of CaF₂:Yb, NaMgF₃Yb and MgF₂:Yb are presented to investigate excitation and relaxation mechanisms of both impurity-trapped excitons and intrinsic excitons in each fluoride host. Host-to-impurity energy transfer mechanisms leading to formation of impurity-trapped excitons are discussed. The 4f¹⁴ → 4f¹³5d CaF₂:Yb²⁺ absorption bands are successfully modeled with a semi-empirical effective Hamiltonian calculation for NaMgF₃:Yb²⁺ and MgF₂:Yb²⁺. The excitation and emission spectra of all studied materials are compared. Results on VUV spectroscopy of 3 and 5 monolayer CdF₂–CaF₂ superlattices show the change in optical behaviour of the self-trapped exciton in CdF₂ when it is confined and give an indication of the radius of the exciton. The decay of the emission is modeled with three components, corresponding to three self-trapped exciton states. Results on the VUV spectroscopy of CdF₂–CaF₂ superlattices show that the confinement effect seems to equally influence the energy of excitonic and bandgap absorption in 3 and 5 monolayer superlattices. At the same time, as the self-trapped exciton is more confined, the emission is blue-shifted by 1600 cm⁻¹ indicating that the effective excitonic radius is about three monolayers.

Depuis les années 1970, le développement des sources lasers de puissance fonctionnant autour de 2 µm basées sur des cristaux dopés Thulium Tm3+ et/ou Holmium Ho3+est un domaine de recherche actif du fait de ses multiples applications. L’émission autour de 1.9 µm correspond à une transition du niveau excité 3F4 vers le niveau fondamental 3H6 dans un ion trivalent Tm3+, alors que l’émission à 2 µm et au-delà correspond à la transition entre le niveau 5I7 et le niveau fondamental 5I8 de l’ion Ho3+. Ces transitions laser font aujourd’hui l’objet de nombreuses applications dans domaines très variés. nous avons étudié les propriétés spectroscopiques de cristaux de fluorures dopés terres rares en vue d’une émission autour de 2 µm. À partir des spectres d’absorption obtenus, l’analyse de Judd-Ofelt a permis de calculer les durées de vie radiatives ainsi que les rapports de branchement dans les ions Tm3+ et Ho3+. En comparaison avec d’autres cristaux tels que les oxydes, les durées de vie des niveau 3F4(Tm3+) et 5I7(Ho3+) dans les cristaux de fluorures sont plus longues ce qui favorise un fonctionnement laser en régime impulsionnel. Une étude sur la dynamique de fluorescence a été réalisée afin de caractériser l’émission autour de 1.9µm de l’ion Tm3+ et celle autour de 2µm de l’ion Ho3+. Les spectres d’émission obtenus offrent de larges bandes, assez structurées dans la matrice LiYF4 et plus larges et moins structurées dans la matrice CaF2. Dans un second temps, en mesurant les durées de vie du niveau émetteur 3F4 pour différentes concentrations en ions Tm3+, nous avons calculé les paramètres de transferts. Les résultats obtenus ont montré que le processus de relaxation croisée est beaucoup plus efficace dans le cristal CaF2 que dans le LiYF4. Nous avons calculé également les coefficients de transfert et de transfert inverse entre les ions Tm3+ et Ho3+ suite à une excitation de l’ion Tm3+. Nous avons montré que la matrice LiYF4 offre une meilleure efficacité de transfert en vue d’une émission autour de 2µm. Le fonctionnement laser de couches minces en configuration « disque mince » a été étudié. Une première démonstration d’un laser en disque mince LiYF4 : Tm émettant à 1.9 µm réalisé à partir d’une couche épitaxiée par LPE a été faite. En simple passge, une puissance de sortie de 306 mW et une efficacité laser de 36% en puissance absorbée sont atteintes pour une couche de 240 μm d'épaisseur.nous avons étudié un oscillateur laser en guide d’onde LiYF4 :Tm en géométrie planaire et linéaire. Ces guides sont caractérisés par de faibles pertes de propagation grâce à la qualité du procédé de fabrication. Une puissance maximale de 470 mW et un rendement de 14% en puissance incidente ont été obtenus. Une modélisation numérique de l’amplification optique montre que le guidage des faisceaux pompe et sonde permet d’atteindre des gains importants. Le modèle est ensuite adapté pour le régime de saturation afin de calculer le rendement d’extraction et de déterminer le potentiel des guides LiYF4 :Tm3+ en tant comme amplificateur autour de 1.9 µm / Since the 1970s, the development of power laser sources operating around 2 μm based on Thulium Tm3 + and / or Holmium Ho3 + doped crystals is an active field of research because of its multiple applications. The emission around 1.9 μm corresponds to a transition from the excited level 3F4 to the fundamental level 3H6 in a trivalent ion Tm3 +, whereas the emission at 2 μm and beyond corresponds to the transition between the level 5I7 and the fundamental level 5I8 of the Ho3 + ion. These laser transitions are today the subject of many applications in a wide variety of fields. We have studied the spectroscopic properties of rare earth doped fluoride crystals for emission around 2 μm. From the absorption spectra obtained, the Judd-Ofelt analysis made it possible to calculate the radiative lifetimes as well as the branching ratios in the Tm3 + and Ho3 + ions. In comparison with other crystals such as oxides, the lifetimes of the 3F4 (Tm3 +) and 5I7 (Ho3 +) levels in the fluoride crystals are longer, which favors pulse-mode laser operation. A study on fluorescence dynamics was carried out in order to characterize the emission around 1.9 μm of the Tm3 + ion and that around 2 μm of the Ho3 + ion. The emission spectra obtained have broad bands, fairly structured in the LiYF4 matrix and wider and less structured in the CaF2 matrix. In a second step, by measuring the lifetimes of the 3F4 emitter level for different Tm3 + ion concentrations, we calculated the transfer parameters. The results obtained showed that the process of cross relaxation is much more efficient in the CaF2 crystal than in LiYF4. We also calculated the transfer and inverse transfer coefficients between Tm3 + and Ho3 + ions following excitation of the Tm3 + ion. We have shown that the LiYF4 matrix offers a better transfer efficiency with a view to emission around 2 μm. The laser operation of thin layers in "thin disc" configuration has been studied. A first demonstration of a thin-film LiYF4: Tm laser emitting at 1.9 μm made from an epitaxial layer with LPE was made. In single passge, an output power of 306 mW and a laser efficiency of 36% in absorbed power are reached for a 240 μm thick layer. We have studied a laser oscillator in LiYF4: Tm waveguide in planar geometry. and linear. These guides are characterized by low propagation losses thanks to the quality of the manufacturing process. A maximum power of 470 mW and a yield of 14% in incident power were obtained. A numerical modeling of the optical amplification shows that the guidance of the pump and probe beams makes it possible to achieve significant gains. The model is then adapted for the saturation regime in order to calculate the extraction efficiency and to determine the potential of the LiYF4: Tm3 + guides as an amplifier around 1.9 μm