Um Amplificador Paramétrico Óptico (optical parametric amplifier - OPA) é uma fonte de luz coerente, de alta qualidade e sintonizável, baseada em processos ópticos não-lineares de segunda ordem. Alguns modelos possuem largura de banda estreita e um amplo intervalo de sintonia, podendo alcançar regiões que vão desde o ultravioleta até o infravermelho médio. A nossa motivação para construir este amplificador paramétrico óptico é sua utilização em experimentos de espectroscopia vibracional de superfícies através do processo óptico não-linear de segunda ordem, geração de soma de frequências (sum-frequency generation - SFG), que é uma técnica que exige fontes sintonizáveis no infravermelho médio e com altas intensidades de pico e largura de banda estreita. O objetivo desse trabalho foi projetar, montar e testar um amplificador paramétrico óptico capaz de produzir pulsos sintonizáveis de alta energia no infravermelho médio (λ ~ 2,5 a 10 μm) a partir de um laser de bombeio que fornece pulsos de 25 ps, com alta energia em λ = 1064 nm. Para obter-se uma geração de infravermelho bastante eficiente, foi proposto um projeto inovador para amplificadores paramétricos de picossegundos, utilizando-se a geração de supercontínuo de luz branca como feixe sinal do estágio de amplificação paramétrica. O pulso de bombeio (λ = 1064 nm) é dividido em duas partes: a primeira, de menor energia, é utilizada para gerar um pulso de alta largura espectral no infravermelho próximo (supercontínuo de luz branca de picossegundos). Uma fração espectral desse pulso é selecionada através de um monocromador e utilizada como semente do estágio de amplificação paramétrica. O cristal amplificador paramétrico (sulfeto de prata e gálio, AgGaS2) é então bombeado pelo restante do pulso de bombeio e simultaneamente amplifica a semente sintonizável no infravermelho próximo e gera um novo pulso de frequência complementar no infravermelho médio. Foram testados vários meios para geração de supercontínuo, mas os melhores resultados foram obtidos em uma cubeta de 10 cm de comprimento com uma mistura de água e água deuterada (3 % em volume de H2O em D2O) e em uma fibra fotônica não-linear com 2 m de comprimento. Usando o supercontínuo como feixe semente, observou-se amplificação paramétrica no caso do feixe gerado na fibra fotônica com um ganho de 260 vezes, mas não com o feixe gerado na mistura de água/água deuterada, presumivelmente pela maior instabilidade desse supercontínuo. / An Optical Parametric Amplifier (OPA) is a tunable light source of high quality, coherent radiation, based on second-order nonlinear optical processes. Some models have a narrow spectral bandwidth and a tuning range from the ultraviolet to the mid-infrared. The motivation for building this optical parametric amplifier is its use in vibrational spectroscopy of surfaces by a second-order nonlinear optical process, sum-frequency generation (SFG), which is a technique that requires tunable sources in the mid-infrared with narrow bandwidth and high peak intensities. The purpose of this work is to design, implement and test an OPA to generate tunable high energy pulses tuneable in the mid-infrared (λ ~ 2.5 to 10 μm) from a pumping laser that provides 25 ps pulses with high energy at λ = 1064 nm. For an efficient mid-infrared generation, we propose an innovative design for picosecond parametric amplifiers, using the near infrared portion of a white-light supercontinuum pulse as the seed beam for the parametric amplifier. The pump pulse (λ = 1064 nm) is divided into two parts: the first one, with lower energy, generates a high spectral width pulse in the near infrared (white-light supercontinuum picosecond pulse). A spectral fraction of this pulse is selected through a monochromator and is used as seed for the parametric amplification stage. The second part of the laser beam pumps the parametric amplifier crystal (silver gallium sulfide, AgGaS2) which simultaneously amplifies the tunable seed beam in the near infrared and generates a new pulse with complementary frequency in the mid-infrared. Several media were tested for supercontinuum generation, but the best results were obtained with a 10 cm long cuvette with a mixture of water and deuterated water (3 % volume of H2O in D2O) and with a 2 m long nonlinear photonic crystal fiber. Using the supercontinuum as a seed beam, we have obtained parametric amplification of the seed generated by the photonic fiber with a gain of 260 times, but not of the beam generated by the water mixture, presumably because of its significantly higher instability.

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Le plus fréquemment, l’interaction laser-matière est étudiée avec des lasers ayant des longueurs d’onde dans l’infrarouge proche (PIR), car ce sont les lasers qui peuvent générer les impulsions les plus intenses. Pour ces lasers, des cibles de densité allant de 0,05 à 2,5 fois la densité critique sont difficiles à créer mais elles offrent des perspectives intéressantes. Dans cette thèse, des jets d’hydrogène ayant de densité dans ce domaine sont utilisées dans le contexte de deux applications :Premièrement, des ions sont accélérées par choc non-collisionnel (collisionless shock acceleration, CSA). Lors de l’interaction d’une impulsion laser PIR avec une cible légè- rement sur-critique, un faisceau de protons est généré. Il est collimé, dirigé vers l’avant et quasiment monoénergetique. Des simulations indiquent que cela est lié à la formation d’un choc non-collisionnel et à l’accélération des protons par ce choc, en sus de leur accélération par le processus standard dit ”target normal sheath acceleration (TNSA)” qui est effectif en face arrière de la cible. Pour beaucoup d’applications, ces faisceaux de particules quasi-monoénergetiques sont plus appropriés que ceux à spectre large qui sont générés de façon routinière par TNSA.Deuxièmement, de l’énergie est transférée d’une impulsion laser (pump) vers une autre en contrepropagation (seed), par rétrodiffusion Brillouin stimulée, dans le régime de couplage fort (strong coupling-SBS), à des densités entre 0,05 et 0,2 fois la densité critique. Pour des impulsions à large bande (60 nanomètres), le rôle de la pré-ionisation sur la propagation et la rétrodiffusion Brillouin spontanée et stimulée est étudié, en incluant l’influence du chirp. Pour des lasers à bande plus étroite, il est démontré que l’impulsion seed peut être amplifiée par des dizaines de milliJoules, et des signatures d’amplification efficace et d’affaiblissement de l’impulsion laser pompe sont trouvées. Ce concept vise à l’amplification des impulsions laser à des puissances au-delà du seuil de dommage des amplificateurs laser basés sur des matériaux solides. / Laser-matter interaction is studied mostly with near-infrared (NIR) lasers as they can generate the most intense pulses. For these lasers, targets between 0.05 to 2.5 times the critical density are challenging to create but offer interesting prospects. In this thesis, novel high-density Hydrogen gas jet targets with densities in this range are used in view of two applications:First, ions are accelerated by collisionless shock acceleration (CSA). Upon interaction of a NIR laser with a slightly overcritical gas jet target, a collimated, quasi-monoenergetic proton beam is generated in forward direction. Simulations indicate the formation of a collisionless shock and acceleration of protons both by the shock and target normal sheath acceleration (TNSA) on the target rear surface under these conditions. These directed, monoenergetic particle bunches are more suitable for many applications than the broadband particle beams already generated routinely.Second, at densities between 0.05 and 0.2 times the critical density, energy is transferred from one laser pulse (pump) to a counterpropagating pulse (seed), via Stimulated Brillouin Backscattering in the strongly-coupled regime (sc-SBS). For the case of broad- band (60 nanometers) pulses, the role of the preionization for pulse propagation and both spontaneous and stimulated Brillouin backscattering are studied, including the influence of the chirp. It is shown that for narrower bandwidths, the seed pulse is ampli- fied by tens of millijoules, and signatures of efficient amplification and pump depletion are found. This concept aims at amplifying laser pulses to powers above the damage thresholds of solid state amplifiers.

Broadband spectral content is required to support ultrashort pulses. However this broadband content is subject to dispersion and hence the pulse duration of corresponding ultrashort pulses may be stretched accordingly. I used a commercially-available adaptive ultrashort pulse shaper featuring multiphoton intrapulse interference phase scan technology to characterise and compensate for the dispersion of the optical system in situ and conducted experimental and theoretical studies in various inter-linked topics relating to the light-matter interaction. Firstly, I examined the role of broadband ultrashort pulses in novel light-matter interacting systems involving optically co-trapped particle systems in which inter-particle light scattering occurs between optically-bound particles. Secondly, I delivered dispersion-compensated broadband ultrashort pulses in a dispersive microscope system to investigate the role of pulse duration in a biological light-matter interaction involving laser-induced cell membrane permeabilisation through linear and nonlinear optical absorption. Finally, I examined some of the propagation characteristics of broadband ultrashort pulse propagation using a computer-controlled spatial light modulator. The propagation characteristics of ultrashort pulses is of paramount importance for defining the light-matter interaction in systems. The ability to control ultrashort pulse propagation by using adaptive dispersion compensation enables chirp-free ultrashort pulses to be used in experiments requiring the shortest possible pulses for a specified spectral bandwidth. Ultrashort pulsed beams may be configured to provide high peak intensities over long propagation lengths, for example, using novel beam shapes such as Bessel-type beams, which has applications in biological light-matter interactions including phototransfection based on laser-induced cell membrane permeabilisation. The need for precise positioning of the beam focus on the cell membrane becomes less strenuous by virtue of the spatial properties of the Bessel beam. Dispersion compensation can be used to control the temporal properties of ultrashort pulses thus permitting, for example, a high peak intensity to be maintained along the length of a Bessel beam, thereby reducing the pulse energy required to permeabilise the cell membrane and potentially reduce damage therein.

Made available in DSpace on 2016-03-15T19:38:52Z (GMT). No. of bitstreams: 1 Henrique Guimaraes Rosa.pdf: 6486656 bytes, checksum: 6fc9fe7875ed2cceb89c9f5179b9f028 (MD5) Previous issue date: 2015-02-25 / Fundo Mackenzie de Pesquisa / In this thesis, we present results on the fabrication, transfer and characterization of chemical vapor deposition (CVD) graphene and exfoliated graphene over glass and optical fiber substrates, to study optical properties of graphene and its application as a saturable absorber for Erbium-doped fiber laser (EDFL). Monolayer CVD graphene and stacked CVD graphene samples were fabricated and characterized, transferred to the transverse face of optical fibers, and a study on the relation between the optical properties of graphene samples and the properties of ultrashort laser pulses generated in (EDFL) was performed. Furthermore, we have developed a technique for transferring exfoliated nanomaterials which allowed us to transfer exfoliated graphene onto optical fiber s faces and align the graphene flake to the fiber core. With this transfer technique it is possible to fabricate samples with controlled number of graphene layers onto optical fiber faces. As application, we demonstrate ultrashort pulse generation in Erbium-doped fiber laser with exfoliated monolayer graphene samples as saturable absorber. This is the first time that ultrashort laser pulses are generated with a single exfoliated monolayer graphene sample. / Nesta tese, apresentamos resultados sobre a fabricação, transferência e caracterização de grafeno CVD (grafeno fabricado por deposição química de vapor chemical vapour deposition) e de grafeno esfoliado em substratos de vidro e em fibras ópticas, para o estudo das propriedades ópticas do grafeno e sua aplicação como absorvedor saturável em laser à fibra dopada com Érbio (EDFL). Foram fabricadas e caracterizadas amostras de grafeno CVD monocamada e de grafeno CVD empilhado, transferidas para a face transversal de fibras ópticas, e com estas amostras foram feitos estudos sobre a relação entre as propriedades ópticas do grafeno e as propriedades de pulsos ultracurtos gerados em EDFL. Além disto, desenvolvemos uma técnica para a transferência de nanomateriais esfoliados que permitiu a transferência de grafeno esfoliado para fibras ópticas e seu alinhamento com o núcleo da fibra. Com esta técnica de transferência é possível fabricar amostras com controlado número de camadas de grafeno em fibra óptica. Como aplicação, demonstramos a geração de pulsos em EDFL com uma amostra de grafeno esfoliado monocamada como absorvedor saturável. Esta é a primeira vez que pulsos ultracurtos são gerados em lasers à fibra com amostra de grafeno esfoliado de uma única camada sobre a face transversal da fibra óptica.

Cette thèse présente l’étude théorique et expérimentale de la génération et de la mise en forme d’impulsions térahertz (THz). Dans un premier temps, nous avons étudié la génération d’impulsions THz par redressement optique d’impulsions laser femtosecondes intenses dans des cristaux semiconducteurs de ZnTe. Nous avons mis en évidence une forte dépendance de l'efficacité de ce processus de génération avec l'intensité de l'impulsion laser génératrice. Ceci se traduit en particulier par un décalage progressif du spectre vers les basses fréquences et par une évolution anormale de l'énergie THz avec l'intensité laser. Ces comportements résultent d'une combinaison de trois phénomènes : la déplétion de l’impulsion laser au cours de sa propagation dans le cristal, l’absorption de l'onde THz par les porteurs libres créés par absorption à deux photons et une modification de la condition d’accord de phase. Dans un deuxième temps, nous avons développé une approche analytique permettant de générer des impulsions THz de formes particulièrement intéressantes pour les expériences de spectroscopie cohérente ou de contrôle cohérent. Nous avons notamment généré des paires d'impulsions verrouillées en phase, des trains d'impulsions, ainsi que des impulsions THz accordables de grande finesse spectrale. Cette technique repose sur le redressement optique d’impulsions laser femtosecondes mises en forme à l’aide d’un masque à cristaux liquides placé dans le plan de Fourier d’une ligne à dispersion nulle. Afin de démontrer la validité de notre approche, nous avons également développé un programme de simulation qui donne des résultats en très bon accord avec l'expérience. / This thesis deals with the theoretical and experimental study of the generation and shaping of terahertz (THz) pulses. At first, we have studied the generation of THz pulses by optical rectification of intense femtosecond laser pulses in semiconductor ZnTe crystals. We have demonstrated a strong dependence of the efficiency of the generation process with the intensity of the laser pulse. This is evidenced by a progressive shift of the spectrum towards lower frequencies and an abnormal evolution of the THz energy with laser intensity. These behaviors result from a combination of three phenomena: the depletion of the laser pulse during its propagation in the crystal, the absorption of THz wave by free carriers created by two-photon absorption and a change of the phase matching condition. Secondly, we have developed an analytical approach to generate THz shaped pulses particularly interesting for coherent spectroscopy or coherent control. In particular, we have generated phase-locked THz pulses pairs, pulse trains and tunable narrow-band THz pulses. This technique is based on optical rectification of shaped femtosecond laser pulses generated by a liquid crystal Fourier filter. To demonstrate the validity of our approach, we have also developed a program giving results in very good agreement with experiment.