La photo-isomérisation par ouverture de cycle du benzopyrane a été étudiée à l'aide de la méthode MCTDH (Multi-Configuration Time-Dependent Hartree). Nous avons introduit différentes stratégies pour contrôler la conversion du benzopyrane en mérocyanine à l'aide d'impulsions laser. Nous avons utilisé un modèle pour le potentiel électronique à six dimensions développé dans le cadre d'un travail antérieur. Le modèle repose sur une généralisation des Hamiltoniens modèles standards pour les couplages vibroniques et utilise les six coordonnées les plus importantes pour le processus. Le principal objectif est de fournir des stratégies de contrôle qui pourront être utilisées par les expérimentateurs par la suite. Plus précisément, nous avons proposé: (i) une technique de type pompe-sonde pour contrôler la photostabilité, (ii) une stratégie en deux étape avec une préexcitation vibrationnel du système,(iii) une stratégie reposant sur un contrôle par effet Stark induit par un laser non-résonant. / The ring-opening photoisomerization of benzopyran, which occurs via a photochemical route involving a conical intersection,has been studied with quantum dynamics calculations using the multi-configuration time-dependent Hartree method (MCTDH). We introduce a mechanistic strategy to control the conversion of benzopyran to merocyanine with laser pulses. We use asix-dimensional model developed in a previous work for the potential energy surfaces (PES) based on an extension of thevibronic-coupling Hamiltonian model (diabatization method by ansatz), which depends on the most active degrees of freedom. The main objective of these quantum dynamics simulations is to provide a set of strategies that could help experimentalists tocontrol the photoreactivity vs. photostability ratio (selectivity). In this work we present:(i) a pump-dump technique used tocontrol the photostability, (ii) a two-step strategy to enhance the reactivity of the system: first, a pure vibrational excitation inthe electronic ground state that prepares the system and, second, an ultraviolet excitation that brings the system to the firstadiabatic electronic state; (iii) finally the effect of a non-resonant pulse (Stark effect) on the dynamics.

Neste trabalho foram realizadas otimizações no processo de fabricação de micro cavidades na superfície do aço DIN 16MnCr5, com o objetivo de reduzir o coeficiente de atrito dinâmico entre duas superfícies. Para a confecção das micro cavidades (dimples) foi utilizado um laser com pulsos ultracurtos, de largura temporal de algumas dezenas de femtossegundos. Além de estudos de variação de fluência do laser, também foi analisado o resultado da utilização de diferentes perfis de energia do feixe. Para a caracterização das micro cavidades, foram utilizadas técnicas como a microscopia eletrônica de varredura, para análise morfológica, interferometria de luz branca e microscopia confocal para análise topográfica, dimensional e perfilométrica. Foram realizados ensaios de desgaste, em tribômetro para análise da variação do coeficiente de atrito após a texturização. Após os ensaios, percebeu-se que a texturização com pulsos ultracurtos apresenta grande vantagem na confecção de micro cavidades devido a precisão e ausência de interação térmica entre o laser e o material. Em relação ao atrito, as amostras texturizadas apresentaram redução da força e do coeficiente de atrito, porém, foram observados sinais de aumento da pressão de contato entre as superfícies. / In this work, optimizations were realized in the dimples manufacturing process on DIN 16MnCr5 steel surface, the target were to reduce the coefficient of dynamic friction between two surfaces. A laser with ultrashort pulses, temporal width of a few tens of femtoseconds, was used to manufacture dimples. In addition to studies of variation of laser beam fluency, the results of the use of different beam energy profiles were also analyzed. For analysis of dimples, techniques such as scanning electron microscopy (SEM), for morphological analysis, white light interferometry and confocal surface microscopy were used for topographic, dimensional and perfilometry. Wear tests were performed to analyze the variation of the friction coefficient in texturing surface. After the tests, it was observed that the texturing with ultrashort pulses presents a great advantage in manufacturing of dimples, due to the precision and absence of thermal interaction between the laser beam and the material. In relation to the friction coefficient, the textured samples presented a reduction of the friction force and consequently of the friction coefficient, but an increase in the contact pressure between the studied surfaces was observed.

Neste trabalho foram realizadas otimizações no processo de fabricação de micro cavidades na superfície do aço DIN 16MnCr5, com o objetivo de reduzir o coeficiente de atrito dinâmico entre duas superfícies. Para a confecção das micro cavidades (dimples) foi utilizado um laser com pulsos ultracurtos, de largura temporal de algumas dezenas de femtossegundos. Além de estudos de variação de fluência do laser, também foi analisado o resultado da utilização de diferentes perfis de energia do feixe. Para a caracterização das micro cavidades, foram utilizadas técnicas como a microscopia eletrônica de varredura, para análise morfológica, interferometria de luz branca e microscopia confocal para análise topográfica, dimensional e perfilométrica. Foram realizados ensaios de desgaste, em tribômetro para análise da variação do coeficiente de atrito após a texturização. Após os ensaios, percebeu-se que a texturização com pulsos ultracurtos apresenta grande vantagem na confecção de micro cavidades devido a precisão e ausência de interação térmica entre o laser e o material. Em relação ao atrito, as amostras texturizadas apresentaram redução da força e do coeficiente de atrito, porém, foram observados sinais de aumento da pressão de contato entre as superfícies. / In this work, optimizations were realized in the dimples manufacturing process on DIN 16MnCr5 steel surface, the target were to reduce the coefficient of dynamic friction between two surfaces. A laser with ultrashort pulses, temporal width of a few tens of femtoseconds, was used to manufacture dimples. In addition to studies of variation of laser beam fluency, the results of the use of different beam energy profiles were also analyzed. For analysis of dimples, techniques such as scanning electron microscopy (SEM), for morphological analysis, white light interferometry and confocal surface microscopy were used for topographic, dimensional and perfilometry. Wear tests were performed to analyze the variation of the friction coefficient in texturing surface. After the tests, it was observed that the texturing with ultrashort pulses presents a great advantage in manufacturing of dimples, due to the precision and absence of thermal interaction between the laser beam and the material. In relation to the friction coefficient, the textured samples presented a reduction of the friction force and consequently of the friction coefficient, but an increase in the contact pressure between the studied surfaces was observed.

Mais recentemente foi proposta uma nova técnica para tratamento de doenças relacionadas à retina humana, utilizando descargas laser na retina com seqüência de pulsos da ordem de 200 \'mü\'s, em substituição ao tratamento convencional que utiliza pulsos longos da ordem de 300 ms. A principal vantagem da nova técnica é a preservação (sem morte celular) do tecido exposto ao laser. Esse trabalho apresenta os mecanismos adotados para o desenvolvimento de um sistema eletrônico de controle de uma cavidade laser em 586 nm, para uso oftalmológico, que objetiva atender o protocolo exigido por essa técnica mais recente. O referido protocolo exige a formação de pulsos rápidos de laser, o que torna vital a velocidade do sistema eletrônico de controle da cavidade laser. Para atender os requisitos do projeto foram implementados dois controladores de corrente em malha fechada PI (Proporcional integrative controller) que trabalham em sincronismo, um controlador de potência óptica em malha fechada PI, e circuitos auxiliares de controle térmico da cavidade laser. Em software foram implementados um PI de potência, com objetivo de tornar a malha de controle estável com o tempo de resposta necessário, e o PI de controle térmico dos elementos da cavidade laser. Os testes realizados do protótipo demonstraram que o sistema de controle atendeu as especificações de projeto, principalmente no que se refere a tempo de resposta do pulso rápido, ponto fundamental na obtenção do protocolo clínico (FastPulse), que esse trabalho objetiva atender. Adicionalmente, o protótipo foi submetido a teste clínico em um paciente, e os resultados demonstraram eficácia no tratamento e ausência de marcas (lesões) na retina. / Recently, scientists have proposed a new technique for treating diseases related to the human retina, which is based on retinal laser discharges using pulse sequence around of 200 \'mü\'s, replacing the conventional treatment using long pulses around of 300 ms. The main advantage of the new technique is the conservation (without cell death) of the area exposed to the laser. This work presents the mechanisms adopted for the development of an electronic control system of a laser cavity at 586 nm for ophthalmic use, which aims to meet the protocol required by this recent technique. The protocol requires the formation of rapid pulses of laser, which makes the electronic control system response velocity of the laser cavity vital to the protocol. To meet the project requirements were implemented two current controllers in closed loop PI (proportional integrative controller) working synchronized, an optical power controller in closed loop PI, and auxiliary circuits for temperature control of the laser cavity. Software were implemented for two controls, a PI power, in order to make the control loop stable with the required response time, and a PI thermal control for elements of the laser cavity. Tests showed that the prototype met the design specifications, especially regarding the response time of rapid pulse, key point in obtaining the clinical protocol (FastPulse), that this work aims to meet. Additionally, the prototype was subjected to clinical trial on a patient, and the results demonstrated efficacy and no visible lesions were noticed on retina.

Die vorliegende Arbeit ist der Verbesserung der Carrier-Envelope Phasenstabilisierung von ultrakurzen Laserimpulsen gewidmet. Zur Realisierung von Fortschritten auf diesem Gebiet werden die grundlegenden Rauschquellen identifiziert, die das erzielbare Restphasenrauschen limitieren, und geeignete Maßnahmen zu deren Verringerung vorgeschlagen. Es wird gezeigt, dass sowohl die Messung der Carrier-Envelope Phase (CEP) als auch deren Kontrolle durch verschiedene Rauschbeiträge beeinträchtigt wird. Der Detektionsprozess ist dabei einerseits durch technische Rauschquellen beeinflusst, die vor allem in den verwendeten nichtlinearen Interferometern auftreten. Andererseits repräsentiert das Detektionsrauschen während der elektro-optischen Wandlung eine fundamentale Limitierung, da das optische Schrotrauschen sowie das Rauschen des Lichtdetektors die Messung der CEP unausweichlich beeinträchtigen. Es wird demonstriert, wie solche Beschränkungen durch geeignete Wahl der Interferometertopologie, bzw. durch Optimierung des spektralen Verbreiterungsmechanismus verringert werden können. Experimentell gelingt es dadurch den Signal-Rauschabstand der Phasenmessung um 20 Dezibel zu steigern. Hinsichtlich der CEP Kontrolle von Oszillatoren wird in dieser Arbeit ein neuartiges Doppelstabilisierungskonzept vorgestellt, welches eine feed-forward Stabilisierung, die auf einem akustooptischen Frequenzschieber beruht, mit einer klassischen Feedback Regelung kombinert. Mit diesem Konzept gelingt eine Reduzierung des Phasenrestrauschen auf beispiellose 20 Milliradian. Darüber hinaus werden weitere neue Stabilisierungskonzepte vorgestellt, die ohne Feedback zu dem Laseroszillator auskommen. Bei einem dieser Konzepte, handelt es sich um eine gepulste feed-forward Stabilisierung, die speziell für das Zusammenwirken mit einer Verstärkerstufe konzipiert ist. Erste experimentelle Ergebnisse zeigen, dass Phasenrestrauschen von weniger als 100 Milliradian auch für Verstärkersysteme erreichbar sind. / The present thesis is dedicated to improvements of the carrier-envelope phase stabilization of ultrashort laser pulses. In order to realize such improvements, the fundamental noise sources are identified, and suitable measures for their reduction are proposed. It is shown that both, the measurement of the carrier-envelope phase (CEP) as well as its control are corrupted by different noise contributions. On the one hand, the detection process is influenced by technical noise sources, which arise especially in the used nonlinear interferometers. On the other hand, the detection noise in the electro-optic conversion represents a fundamental limitation, since the optical shot noise as well as the noise induced by the light detector inevitably influence the measurement of the CEP. It is demonstrated how such limitations can be minimized by a suitable choice of the interferometer topology and by an optimization of the spectral broadening process in a micro-structured fiber. This way an enormous improvement of the signal-to-noise ratio by 20 dB is obtained experimentally, which significantly reduces the limitation of detection noise. For controlling the CEP of mode-locked oscillators, a novel double stabilization scheme is introduced in this thesis, which combines a feed-forward stabilization based on an acousto-optic frequency shifter, with a classical feedback loop. This method enables a reduction of the residual phase jitter to an unprecedented value of 20 milliradian. Beyond that, several further concepts are introduced that are capable of stabilizing the CEP without any feedback to the laser oscillator. One of these concepts, represents a pulsed feed-forward stabilization, which is specifically designed for the use in combination with a subsequent amplification stage. First experimental results indicate that residual phase jitters of less than 100 milliradian are within reach also for amplified laser systems.

In this Thesis, two problems were studied: a direct vacuum acceleration of electrons by a tightly focused ultrashort relativistic laser pulse and ion acceleration in the process of spherical laser-heated plasma explosion. The electromagnetic field of a tightly focused laser pulse was evaluated numerically by means of Stratton-Chu integrals. The properties of the focused field were analyzed in detail for a plane wave or a macroscopically large Gaussian beam incident onto the mirror. Free electrons moving in the tightly focused field were found to accelerate by two possible mechanisms: focal spot acceleration and capture-and-acceleration scenario. The two mechanisms were studied in detail. Comparison of the mirror-focused field with first- and fifth-order paraxial fields is performed. A 3D electromagnetic PIC code SCPIC was created for simulations of pulse interaction with targets having a finite number of particles interacting with each other by collective fields. Atto-second bunch formation was observed in the interaction with ultra-small or ultra-thin targets. Physical mechanism of bunch formation is explained. The problem of electrostatic explosion of a nano-scale spherical plasma with initially hot electrons and cold ions was solved numerically. Expansion in a wide regime of electron temperature $0 < T leq infty$ was studied in detail for different initial density profiles of plasma. Favorable conditions for obtaining mono-energetic ions resulting from the explosion were specified in single and two ionic species cases. In case of a two-species explosion, the number of mono-energetic, $deltavarepsilon/varepsilon < 10\%$, ions can be as high as 70-80\% of the total light ions for a wide range of electron temperatures.

Many essential processes and interactions on atomic and molecular scales occur at ultrafast timescales. The ability to measure and manipulate ultrashort pulses hold the key to probing and understanding these key processes that physicists, engineers, chemists and biologists study today. Measuring ultrashort pulses means that we measure both the intensity (which is a function of time) and the phase of the pulse in time. Or alternately we might measure spectrum and spectral phase (in the corresponding Fourier domain). In the early 1990's, the invention of FROG opened up the field of ultrashort measurement with it's ability to measure the complete pulse. Since then, there have been a whole host of pulse measurement techniques that have been invented to measure all sorts of ultrashort pulses. However, no variation of FROG nor any other fs pulse measurement technique, for that matter, has yet been able to completely measure arbitrary ultraweak femtosecond light pulses such as those found in nature. In this thesis, we will explore a couple of highly sensitive methods in a quest to measure ultraweak ultrashort pulses. We explore the use of Spectral Interferometry, a known sensitive technique as one possibility. We find that it has certain drawbacks that make it not necessarily suitable to tackle this problem. But in the course of our quest, we find that this technique is highly suitable for measuring 10s of picosecond-long shaped pulses. We discuss a couple of developments which make SI highly practical to use for such shaped pulse-measurements. We also develop a new technique which is a variation of FROG, based on the non-linearity of Difference Frequency Generation and Optical Parametric Amplification, which can amplify pulses as weak as a few hundred attojoules to be able to spectrally resolve them and measure the full intensity and phase of these pulses. This technique offers great potential to measure generalized ultraweak ultrashort pulses.

No description available.

The purpose of this thesis is to advance the understanding of strong-field QED processes in short laser pulses. The processes of non-linear one-photon and two-photon Compton scattering are studied, that is the scattering of photons in the interaction of relativistic electrons with ultra-short high-intensity laser pulses. These investigations are done in view of the present and next generation of ultra-high intensity optical lasers which are supposed to achieve unprecedented intensities of the order of 10^24 W/cm^2 and beyond, with pulse lengths in the order of some femtoseconds. The ultra-high laser intensity requires a non-perturbative description of the interaction of charged particles with the laser field to allow for multi-photon interactions, which is beyond the usual perturbative expansion of QED organized in powers of the fine structure constant. This is achieved in strong-field QED by employing the Furry picture and non-perturbative solutions of the Dirac equation in the presence of a background laser field as initial and final state wave functions, as well as the laser dressed Dirac-Volkov propagator. The primary objective is a realistic description of scattering processes with regard to the finite laser pulse duration beyond the common approximation of infinite plane waves, which is made necessary by the ultra-short pulse length of modern high-intensity lasers. Non-linear finite size effects are identified, which are a result of the interplay between the ultra-high intensity and the ultra-short pulse length. In particular, the frequency spectra and azimuthal photon emission spectra are studied emphasizing the differences between pulsed and infinite laser fields. The proper description of the finite temporal duration of the laser pulse leads to a regularization of unphysical infinities (due to the infinite plane-wave description) of the laser-dressed Dirac-Volkov propagator and in the second-order strong-field process of two-photon Compton scattering. An enhancement of the two-photon process is found in strong laser pulses as compared to the corresponding weak-field process in perturbative QED.

Se describe la aplicación de pulsos láser ultracortos (≤10fs) en espectroscopía y microscopía de dos fotones llevada a cabo en nuestro grupo de investigación, subrayando las ventajas y requerimientos de este enfoque. Además se presenta una breve descripción de la manipulación de pulsos, de las distorsiones de fase experimentadas por los pulsos láser de femtosegundo y de cómo corregir tales distorsiones utilizando manipuladores de pulsos. / Femtosecond laser pulses in two-photon spectroscopy and microscopy: The application of shaped ultrashort laser pulses (≤10fs) in two-photon spectroscopy and microscopy carried out in our group is  described, highlighting the advantages and requirements of this approach. In addition, a brief description of pulse shaping, phase distortions experienced by femtosecond laser  pulses and how to correct these distortions using a pulse shaper is also presented.