Neste trabalho foi estudada a geração de harmônicos perturbativos por pulsos laser ultracurtos em bicos de gás no vácuo. Os harmônicos foram gerados nas regiões espectrais do UV e VUV e sua geração ocorreu em fluxo de gases nobres. Esta técnica possibilita a produção de luz coerente numa região espectral de interesse considerável para várias aplicações, tais como a espectroscopia resolvida no tempo. Para a geração dos harmônicos foi utilizado um sistema laser amplificado de Ti:Safira que produz pulsos de 25 fs, centrados em 785 nm, a 4 kHz. Estes pulsos ultracurtos são injetados em uma câmara de vácuo, onde são focalizados em um bico de gás. Os harmônicos são selecionados por um monocromador e têm a sua intensidade medida por um cintilador e uma fotomultiplicadora. Buscamos abranger uma visão geral sobre a geração de harmônicos perturbativos em gases, com o objetivo de consolidar um conhecimento teórico e experimental no laboratório. Confeccionamos e comparamos o desempenho de dois sistemas distintos de injeção de gás, o bico metálico e o bico de vidro, que são dispositivos pouco explorados na literatura. Os melhores resultados foram obtidos com o bico de vidro. Pudemos estimar a eficiência de geração dos harmônicos do ponto de vista das propriedades microscópicas e macroscópicas de geração, e foi verificada a conversão de energia do feixe fundamental para a geração dos harmônicos, plasma e outros fenômenos não-lineares em argônio. Geramos até o 9º harmônico em argônio, atingindo a região de 85 nm. Foi estudado o casamento de fase e a dependência da eficiência de geração dos harmônicos com a pressão do gás, potência média do laser, chirp e a posição do foco para o 3º, 5° e 7º harmônicos. Com a variação dos parâmetros, observou-se que é possível sintonizar os harmônicos, e que sua geração compete com outros fenômenos, como a ionização do gás. Adicionalmente, foi observada uma queda da eficiência de geração para alta intensidades, que foi associada à depleção do 1º elétron de valência dos átomos do gás, reduzindo a quantidade de centros geradores dos harmônicos. Além do argônio, foram realizadas medidas em hélio, neônio e criptônio, visando estudar como a eficiência de geração dos harmônicos depende das propriedades eletrônicas do gás. Adicionalmente, esses resultados corroboraram a hipótese da depleção dos elétrons de valência. / In this work the generation of perturbative harmonics by ultrashort laser pulses in gas nozzles in vacuum was studied. The harmonics were generated in the UV and VUV regions and the frequency conversion occurred in flowing gas. This technique ensures the generation of coherent light in a spectral region of interest for various applications, such as ultrafast time-resolved spectroscopy. For the harmonics generation an amplified Ti:Shapphire laser system was used, generating 25 fs pulses, centered at 785 nm, at 4 kHz. These ultrashort pulses are injected into a vacuum chamber, where they are focused on a gas nozzle. The harmonics are selected by a monochromator and their intensity is measured by a scintillator and photomultiplier. We have sought to comprise an overview of the generation of perturbative harmonics in gases, in order to consolidate a theoretical and experimental knowledge in the laboratory. Two distinct gas injection systems were manufactured and had their performances compared, a metallic and a gas nozzle, devices that are poorly explored in literature. The best results were obtained with the glass nozzle. We could estimate the harmonics generation efficiency in argon from the point of view of their macroscopic and microscopic generation properties, and the energy conversion from the fundamental beam to the harmonics was verified, along with plasma creation and other nonlinear phenomena. We generated up to the 9th harmonic in argon, reaching the 85 nm. We studied the phase matching and the dependence of the harmonics generation efficiency with the gas pressure, laser average power, chirp and focus position for the 3rd, 5th and 7th harmonics. By varying the parameters, we observed that it is possible to tune the harmonics wavelengths, and that their generation competes with other nonlinear phenomena, such as the gas ionization. Additionally, a drop in the generation efficiency was observed at high intensities, which was associated to the depletion of the first valence electron in the gas atoms, decreasing the number of harmonic generating centers. In addition to argon, measurements were performed in helium, neon and krypton, aiming to study how the harmonic generation efficiency depends on the electronic properties of the gas. Additionally, these results corroborated the hypothesis of the valence electron depletion.

Em sólidos dopados com Cr+3, o efeito não-linear ocorre devido à população de íons dopantes no estado metaestável, o qual possui uma polarizabilidade diferente do estado fundamental. Nestes materiais, o índice de refração não-linear n2 é proporcional a Δα/Is , onde Δα é a diferença de polarizabilidade, entre os estados, excitado (metaestável) e o fundamental, e Is a intensidade de saturação da transição. A técnica conhecida como Z-Scan é na atualidade a mais popular para medidas de n2 e foi recentemente aplicada em cristais dopados com Cr+3. Nestes materiais, o tempo de resposta do meio não-linear é dado pelo longo tempo de vida espontâneo do estado excitado τ0 (usualmente τ0 > 100 µs) tornando possível medidas da resposta transiente do sinal. Isto torna possível a normalização do sinal pela medida em t =O (quando o efeito não-linear ainda não se manifestou) com o intuito de eliminar efeitos lineares parasíticos (devido a imperfeições da superfície da amostra, não paralelismo, etc.). Neste trabalho 7 nós usamos o método de Z-Scan resolvido no tempo para determinar não apenas n2, mas também a intensidade de saturação Is. Nós introduzimos um novo método para determinação de Is, através da medida de Z-Scan transiente. Os valores de n2 e Is, podem ser usados para calcular a seção de choque da absorção no estado fundamental σ1, Δα e Δσ (a diferença de seção de choque de absorção entre o estado excitado e metaestável). , Fizemos medidas em cristais de rubi e alexandrita usando um laser de Ar modulado por um \"chopper\". No caso da alexandrita, o Cr+3 pode ocupar dois sítios que apresentam propriedades bastante diferentes. A técnica resolvida no tempo permite que se diferencie estes dois sítios, e então se determine n2, Is, τ0, Δα e Δσ para o íon de Cr+3 em cada tipo de sítio (no caso do sítio de espelho os valores de n2 e Δα são inéditos). / In Cr+3 doped solids, the nonlinearity originates from the population of dopant íon metastable excited state, which has a polarizability different from that of ground state. In these materials, the non-linear refractive index n2 is proportional to a Δα/Is, where a Δα is polarizability difference between excited and ground states and Is is the transition saturation intensity. The thecnique known as Z-Scan is nowadays the most popular one for n2 measurements and was recently applied to Cr+3 doped solids. In this material, the nonlinearity response time is given by the excited state spontaneous lifetime τ0 (usually τ0 > 100 µs) permitting transient response measurements. This allows signal normalization at t=0 (when the nonlinear effect did not appear yet) in order to eliminate parasitic linear effects (due to nonparallel sample surfaces, surface imperfections, etc.). In the present work we used a time resolved Z-Scan method to determine not only n2 but also the saturation intensity Is and these values can be used to calculate the ground state absorption cross section σ1, Δα and Δσ (where Δσ is the absorption cross section difference between excited and ground states). We introduced a new method to measure Is through transient Z-Scan measurements. We performed measurements in ruby and alexandrite using a chopped Ar+ ion laser. In the alexandrite crystal the Cr+3 ion can occupied two different sites that have very different spectroscopy properties. The time resolved technique allowed us to distinguished these two sites and then determine n2, σ0, Δα , Δσ and Is for the Cr+3 ion each kind of site(our n2, Δα and Is results for the mirror site are original contributions of these work).

Neste trabalho nós crescemos e caracterizamos oticamente cristais de L-treonina e L-lisina-HCl. Esses materiais pertencem a uma família de cristais orgânicos que tem demonstrado potencial para uso como dispositivos ópticos não lineares. Os cristais foram crescidos em solução aquosa pelos métodos de evaporação lenta do solvente e abaixamento controlado da temperatura. Realizamos medidas de óptica linear, índices de refração e a absorção óptica, e de óptica não linear, a geração de segundo harmônico (GSH). Essa nova classe de materiais não linear é de fácil crescimento e apresentam uma boa qualidade óptica e propriedades não lineares comparáveis as dos cristais de KDP. / In this work we grew and optically characterized L-threonine and L-lysine-HCL crystals. These materials belong to a family of organic crystals that have a potential application in nonlinear optical devices. The crystals were grown in aqueous solution by slow solvent evaporation and controlled cooling techniques. We characterized the linear and nonlinear optical properties of these materials, for exarnple, the index of refi-action, optical absorption and second harmonic generation (SHG). This new class of nonlinear medium is easy to grow and present good optical quality and nonlinear properties comparable to KDP crystals.

Au cours de cette thèse, nous avons synthétisé de nouveaux composés en utilisant des macrocycles de porphyrines comme socle pour nos architectures. L'objectif était d'étudier leurs propriétés en optique linéaire et non linéaire. Plus précisément, nous avons synthétisé et caractérisé trois groupes de dendrimères de type fluorényl-porphyrine, une série de porphyrines organométalliques dérivés du ruthénium, et commencé une dernière série de nouvelles porphyrines. Les corrélations entre les propriétés et la structure ont été étudiés, le processus de transfert d'énergie du donneur vers la porphyrine a aussi été évalué. En introduction, nous avons présenté le contexte général de la chimie des porphyrines basé sur quatre aspects: (1) la structure chimique, (2) les voies de synthèse, (3) les propriétés en optique linéaire (4) et en optique non linéaire. Nous avons ensuite présenté les différents travaux qui ont été effectués dans notre groupe, et conclut en proposant de nouvelles structures basées sur ces résultats. Dans le premier chapitre, nous présentons la synthèse d'un groupe de dendrimères dérivés de thiényl-porphyrines. Les unités thiényles font le pont entre les dendrons conjugués de type fluorényle et le coeur de la porphyrine. Le transfert d'énergie pour ces molécules est efficace et ces dernières présentent des propriétés en optique non linéaire qui sont intéressantes avec une amélioration de l'absorption à deux photons (ADP). Dans le deuxième chapitre, nous présentons la synthèse d'une série de composés à base de ruthénium dérivés de la Tétrafluorényl- porphyrine (TFP), pour des applications en optique non linéaire (üNL). Dans le troisième chapitre, nous présentons la synthèse de deux nouveaux dendrons avec des antennes fluorényles terminales greffées en position 9 d'un troisième fluorényle, respectivement par voie conjuguées ou non conjuguées. Puis deux nouveaux dendrimères ont été obtenus par couplage de Sonogashira à partir de ces dendrons sur le coeur porphyrine TFP. Le transfert d'énergie de ces dendrons vers la porphyrine est efficace. Ces molécules présentent des propriétés en optique non linéaire qui sont intéressantes et les résultats en ADP sont très prometteurs. Dans le quatrième chapitre, nous présentons la synthèse de porphyrines avec des bras fluorénones terminales. Ces porphyrines émettent également une luminescence rouge et le transfert d'énergie est très efficace. Comme perspectives, un nouveau type de porphyrine méso-alcynyle est envisagé, pour l' instant nous avons juste synthétisé la génération 0 de cette série de dendrimères: Les quatre bras tluorényles sont pontés au coeur de la porphyrine avec des liens alcynyles, et les études optiques de ces prototypes sont en cours. / During this thesis, we have elaborated new compounds using the porphyrin macrocycle as the basic platform of our architectures. The aim, after their syntheses, was to study the linear optical (LO) and non-linear optical (NLO) properties of these new molecules. More precisely, we have synthesized and characterized three groups of fluorenyl-porphyrin dendrimers, a series of ruthenium organometallic porphyrins, and started a series of new type of porphyrin. Their correlations on optical property-structure have been discussed, as well as the energy transfer processes from the donor fragments to porphyrin core acceptor. In the introduction, we presented the general background of the porphyrin chemistry based on four aspects: ( I) structure, (2) synthetic methods, (3) LO properties and (4) NLO properties. We further reviewed prior porphyrin studies done in our group and proposed new molecular designs based on these results. In the first chapter, we synthesized a group of thienyl porphyrin cored dendrimers. The thienyl units connect the conjugated fluorenyl dendrons to porphyrin ring by alkynyl bridges. The energy transfer (ET) of these porphyrins is very efficient and they present interesting NLO properties with enhanced Two-photon absorption (TPA). In the second chapter, we synthesized a series of ruthenium compounds based on Tetra-fluorenyl porphyrin core (TFP) for NLO applications. In the third chapter, we synthesized two new dendrons with two terminal fluorenyl antennae fi xed on the 9 position of the fluorenyl units in conjugated or non-conjugated way respecti vely. Then two new porphyrin dendrimers were obtained by Sonogashira coupling reaction of these dendrons on TFP porphyrin core. Their ET from dendrons to porphyrin core is very efficient. They present interesting LO properties and the TPA results are very promising. In the fourth chapter, we synthesized a group of TFP cored porphyrins with terminal fluorenone anns. These porphyrins emit red luminescence and the ET is very efficient from the linear arms toward their cores. As perspective, a new type of meso-alkynyl porphyrin series is considered, for the moment we synthesized only the generation 0 of the dendrimers: the four fluorenyl arms of this porphyrin are bridged to the centre ring by alkynyl chains, and the optical studies of this prototype are in progress.

The Optical Parametric Oscillator (OPO) has been one of the most versatile source of non-classical states of light. Usual configurations of such devices are a macroscopic second order nonlinear crystals inside an optical cavity. Recently the use of silicon photonics techniques allowed the implementation of high quality factor microcavities and OPOs which include several technological advantages over usual configuration as a small size, bigger bandwidth, CMOS compatibility, facility to engineer the dispersion properties and compatibility with commercial optical fiber communications. Nevertheless the nonlinearity present within these systems is a third order nonlinearity for which theoretical calculations lack in the literature. Here we describe theoretically the quantum properties of the light generated in an OPO with a third order nonlinearity. We showed that the effects of phase modulation (which are not present in the second order nonlinearity) and dispersion are determinant in the way that oscillation and entanglement is produced in the system. Despite of these effects, bipartite and tripartite entanglement is predicted with the use of the Schmidt modes formalism. We also describe the system when there are more modes exited within the cavity and a frequency comb is formed. In such a situation, using again the Schmidt modes formalism, multipartite entanglement was predicted as well. / O oscilador paramétrico ótico (OPO) tem sido uma fonte muito versátil de estados não clássicos da luz. A configuração usual destes OPOs consiste em um cristal macroscópico com não linearidade de segunda ordem no interior de uma cavidade ótica. Recentemente, devido ao desenvolvimento da fotonica de silício, foi possível a implementação de micro- cavidades óticas e OPOs que possuem varias vantagens sobre OPOs usuais. Não entanto a não linearidade destes sistemas é de terceira ordem. Neste trabalho, descrevemos teoricamente as propriedades quânticas da luz gerada num OPO com não linearidade de terceira ordem. Mostra-se que os efeitos de modulação de fase (não presentes na não linearidade de segunda ordem) e a dispersão são determinantes para a geração e o emaranhamento produzido no sistema. Emaranhamento bi e tri partito foi predito teoricamente usando o formalismo de modos de Schmidt. Também foi feita uma descrição quando mais modos da cavidade são excitados gerando um pente de frequência. Nesta situação. e utilizando novamente o formalismo de modos de Schmidt, foi predito emaranhamento multimodo destes sistemas.

The preparation of single photons in a pure quantum state is a subject of great interest in physics, enabling the control of light at an unprecedented level. The ease with which certain degrees of freedom of photon states, such as polarisation, can be manipulated, along with the inherent resilience of photons to decoherence, makes them well suited for use as qubits. Recent rapid developments in the transmission and processing of quantum information, as well as the likely technological impact of potential real-world applications such as quantum cryptography and quantum computation, mean that the demand for high performance single photon sources is likely to increase in the near future. One approach to producing single photon states, which are known to be in a well-defined spatio-temporal mode without destructively measuring them, is to take advantage of nonlinear optics. Nonlinear processes can be used to realise frequency conversion by generating a single, correlated pair of photons from an intense pump laser source. The detection of one of the photons from a pair can then be used to indicate the presence of the other photon in the pair, a procedure known as heralding. This thesis describes the development of a source of heralded single photons at 1550 nm, generated directly in the core of a photonic crystal fibre (PCF). By taking advantage of low loss fibre components for the required spectral filtering of the generated photon state, a heralding fidelity of 52% was achieved. The source was designed to be used with a picosecond pulsed fibre laser, making it relatively low cost and maintenance free. With 148 mW of average pump power a heralded output photon rate of 6.4 × 104 s-1 was observed, demonstrating the brightness of the source. The purity of the generated single photons was established by measuring non-classical interference, with a visibility of 70%, between the photons output from this source and a source based on a PPLN waveguide. The fabrication of a series of birefringent PCFs for the generation of spectrally pure state photons at 1550 nm is also discussed. These PCFs will be useful for incorporation in the next generation of high performance, fibre-based photon sources.

No description available.

De nombreuses applications militaires ou civiles, telles que la spectroscopie dans les bandes de transmission de l’atmosphère (bandes 3-5µm et 8-12µm), nécessitent de disposer de sources émettant dans le moyen infrarouge (IR). Les travaux de cette thèse portent sur la génération de rayonnement dans la bande 3-5µm par amplification paramétrique (mélange à quatre ondes) dans les fibres optiques en verres fluorés et en verres de chalcogénures. La première partie de ce travail a été consacrée à l’étude théorique et à la modélisation des conditions d’accord de phase et du gain paramétrique dans des fibres à saut d’indice monomodes en verres fluorés ZBLAN et verres de chalcogénures As2S3 et As2Se3. La nature des résultats obtenus nous a conduit à étudier théoriquement le potentiel de l’accord de phase multimode dans les fibres en verres de chalcogénures. La deuxième partie de ce travail a porté sur la modélisation de l’amplification paramétrique dans des fibres en verres de chalcogénures microstructurées à géométrie hexagonale. Pour ce faire, un modèle simplifié de la propagation dans les fibres microstructurées hexagonales a été développé : le modèle de l’indice effectif de gaine (EIM). Il a ensuite été comparé à une méthode de résolution aux éléments finis. Grâce à cette comparaison, nous avons pu améliorer la précision du modèle EIM en déterminant la valeur de plusieurs paramètres empiriques. Ce modèle nous a alors permis de prédire l’efficacité du processus d’amplification paramétrique dans les fibres microstructurées. L’ensemble de ces études théoriques a permis d’identifier les fibres les plus adaptées à la conversion de fréquence vers la bande 3-5µm. Enfin, nous avons réalisé un banc de mesure de la dispersion chromatique des fibres, ainsi que le dimensionnement d’un convertisseur de fréquence utilisant les fibres identifiées dans l’étude théorique. / Various civil or military applications, such as spectroscopy in the atmospheric transparency windows (3 – 5 µm and 8 – 12 µm ranges), require the use of mid-infrared emitting laser sources.The work presented in this thesis is about light generation in the 3 – 5 µm range by parametric amplification (four-wave mixing) in fluoride and chalcogenide fibers. The first part of the study is devoted to modelizations of phase-matching condition and parametric gain in monomode step-index ZBLAN fluoride fibers as well as As2S3 and As2Se3 chalcogenide fibers. The results obtained in this modelization led to the theoretical study of multimode phase-matching conditions in chalcogenide fibers.The second part of the study presents the modelization of parametric amplification in hexagonal microstructured chalcogenide fibers. A simplified model, called the effective index method (EIM), has been developed and compared to the finite element method. Thanks to this comparison, the accuracy of the EIM model was improved through the determination of several empirical parameters. Using the improved EIM model, we have been able to predict the parametric amplification efficiency in microstructured fibers. Thus, all those theoretical studies allowed us to identify the most adapted fibers for frequency conversion in the 3 – 5 µm range. Eventually, we realized an experimental bench to measure the chromatic dispersion of optical fibers, and we suggested an experimental architecture using the fibers we had indentified in the theoretical study.

Lam Sio Kuan. / Thesis (Ph.D.)--Chinese University of Hong Kong, 1998. / Includes bibliographical references (p. 111-116). / Electronic reproduction. Hong Kong : Chinese University of Hong Kong, [2012] System requirements: Adobe Acrobat Reader. Available via World Wide Web. / Mode of access: World Wide Web. / Abstracts in English and Chinese.

Geração de luz supercontínua é um efeito caracterizado por um forte alargamento espectral induzido por efeitos não-lineares no meio óptico, e que encontra uma vasta gama de aplicações, como tomografia por coerência óptica, espectroscopia e metrologia de freqüência. No presente trabalho, os fenômenos físicos responsáveis pela geração de luz supercontínua são estudados teoricamente, utilizando a ferramenta numérica desenvolvida para dar suporte à teoria. Os efeitos de polarização relacionados à geração de luz supercontínua também são analisados e, neste contexto, a utilização de uma fibra de cristal fotônico com formato tipo-D e alta birrefringência é proposta para servir como meio óptico. As características do supercontínuo gerado nesta fibra são analisadas teoricamente, novamente com o apoio da ferramenta numérica. A análise conclui que a fibra proposta apresenta consideráveis vantagens em relação às fibras convencionais, principalmente por ser capaz de manter o estado de polarização da luz supercontínua estável. / Supercontinuum generation is an effect characterized by a strong spectral broadening induced by nonlinear effects in the optical medium. There is a wide range of applications for this effect, such as optical coherence tomography, spectroscopy and frequency metrology. In this work, the physical phenomena responsible for supercontinuum generation are theoretically studied relying on the developed numerical tool to support the theory. The polarization effects related to supercontinuum generation are also assessed and, in this context, a highly birefringent D-shaped photonic crystal fiber is proposed as a medium for supercontinuum generation. The characteristics of supercontinuum generation in the proposed fiber are theoretically analyzed. The analysis concludes that the proposed fiber shows considerable advantages over conventional fibers, mainly due to the capability to keep the state of polarization of the supercontinuum stable.