No description available.

The multiconfiguration time-dependent Hartree-Fock (MCTDHF) and multiconfiguration time-dependent Hartree (MCTDH) methods are employed to investigate nonperturbative multielectron dynamics in finite quantum systems. MCTDHF is a powerful tool that allows for the investigation of multielectron dynamics in strongly perturbed quantum systems. We have developed an MCTDHF code that is capable of treating problems involving three dimensional (3D) atoms and molecules exposed to strong laser fields. This code will allow for the theoretical treatment of multielectron phenomena in attosecond science that were previously inaccessible. These problems include complex ionization processes in pump-probe experiments on noble gas atoms, the nonlinear effects that have been observed in Ne atoms in the presence of an x-ray free-electron laser (XFEL) and the molecular rearrangement of cations after ionization. An implementation of MCTDH that is optimized for two electrons, each moving in two dimensions (2D), is also presented. This implementation of MCTDH allows for the efficient treatment of 2D spin-free systems involving two electrons; however, it does not scale well to 3D or to systems containing more that two electrons. Both MCTDHF and MCTDH were used to treat 2D problems in nanophysics and attosecond science. MCTDHF is used to investigate plasmon dynamics and the quantum breathing mode for several electrons in finite lateral quantum dots. MCTDHF is also used to study the effects of manipulating the potential of a double lateral quantum dot containing two electrons; applications to quantum computing are discussed. MCTDH is used to examine a diatomic model molecular system exposed to a strong laser field; nonsequential double ionization and high harmonic generation are studied and new processes identified and explained. An implementation of MCTDHF is developed for nonuniform tensor product grids; this will allow for the full 3D implementation of MCTDHF and will provide a means to investigate a wide variety of problems that cannot be currently treated by any other method. Finally, the time it takes for an electron to tunnel from a bound state is investigated; a definition of the tunnel time is established and the Keldysh time is connected to the wavefunction dynamics.

O propósito principal desta tese foi a implementação e estudo da geração de pulsos laser de femtossegundos em comprimentos de onda curtos (ultravioleta profundo, ultravioleta de vácuo e ultravioleta extremo) pela técnica de conversão de frequência em capilar preenchido com gás nobre. Esta técnica de conversão de frequência tem feito diversas contribuições nas últimas décadas para o avanço da geração de pulsos laser ultracurtos nesta região espectral. O desenvolvimento de tais fontes de luz coerente possui importantes implicações nos estudos de espectroscopia resolvida no tempo em átomos, moléculas e materiais. Através da implementação da técnica de conversão de frequência com casamento de fase em capilar preenchido com gás argônio, foi possível a obtenção de pulsos de femtossegundos centrados em 260 nm e 195 nm utilizando um sistema laser amplificado Ti: safira (780 nm, 1.5 mJ, 43 fs, 1 KHz). Estes comprimentos de onda correspondem, respectivamente, aos terceiro e quarto harmônicos da frequência fundamental do laser utilizado. Pulsos centrados em 260 nm com excelente perfil espacial, energias da ordem de microjoules e durações temporais tão curtas quanto 18 fs, possibilitadas pela recompressão por um par de prismas, foram obtidos, os quais possuem grande aplicabilidade em estudos de espectroscopia não linear e resolvida no tempo. Pulsos ultracurtos centrados em 195 nm também foram obtidos. Uma investigação da influência da modulação da fase espectral do pulso laser em 780 nm sobre a geração de harmônicos através do processo do mistura de quatro ondas, também foi realizada. Desta forma, foi implementado um sistema de controle de formato de pulso laser de femtossegundo na configuração 4f baseado em um modulador espacial de luz de cristal líquido com o objetivo de modular a fase espectral dos pulsos laser em 780 nm. Este sistema de controle de formato de pulso foi então integrado ao sistema de geração de pulsos ultracurtos no ultravioleta profundo através do processo de mistura de ondas já implementado. Este estudo teve como objetivo, a obtenção da modulação indireta da fase espectral de pulsos em 260 nm através da transferência de fase espectral modulada de pulsos em 780 nm. Resultados iniciais interessantes foram obtidos utilizando uma fase espectral do tipo degrau com amplitude radianos, indicando a correta implementação do sistema. A obtenção de pulsos laser de femtossegundos no ultravioleta profundo com fase espectral modulada é de grande interesse para realização de experimentos de controle coerente nesta região espectral e também para estudos básicos de como a transferência de fase espectral ocorre para diferentes processos ópticos não lineares. Experimentos de geração de altos harmônicos pela técnica de conversão de frequência com casamento de fase em capilar preenchido com gás nobre, utilizando pulsos laser de femtossegundos em 400nm e 800nm, foram realizados durante estágio na Universidade do Colorado, EUA. Neste estudo, utilizando pulsos em 400nm, foi obtido um aumento maior que uma ordem de grandeza na região espectral em torno de 60eV em comparação com o fluxo de harmônicos gerados, nesta mesma região de energia, com pulsos centrados em 800nm. Por fim, através da experiência adquirida durante este estágio, foi desenvolvido e implementado em nosso laboratório um sistema de geração de altos harmônicos na região do ultravioleta extremo, baseado na técnica de conversão em capilar preenchido com gás argônio. Harmônicos de alta ordem na região de energia de 40ev (31nm) foram obtidos, tendo sido demonstrada a conversão sob condição de casamento de fase. Utilizando pulsos de femtossegundos em 780nm, a ordem máxima do harmônico observada foi igual a 27 (28.9nm, 42.9eV), devido a limitação da faixa espectral do monocromador utilizado em nossos experimentos. A implementação deste sistema torna disponível no Grupo de Fotônica, uma fonte de luz coerente no ultravioleta extremo, cujas propriedades únicas já tem sido amplamente exploradas em uma variedade de estudos de ciência básica e aplicada. / The main purpose of this thesis was the implementation and study of femtosecond laser pulses generation at short wavelengths (deep ultraviolet, vacuum ultraviolet end extreme ultraviolet) by the technique of frequency conversion in a hollow fiber filled with a noble gas. This frequency conversion technique has made several contributions in the last decades to improve the generation of ultrashort laser pulses in this spectral region. The development of such coherent light sources has important implications on ultrafast time-resolved spectroscopic study of atoms, molecules and materials. Through the implementation of the technique of phase matched frequency conversion in a gas filled hollow fiber using argon, it was possible to obtain femtosecond pulses centered at 260 nm and 195 nm using a Ti: sapphire amplified laser (780 nm, 1.5 mJ, 43 fs, 1 KHz). These wavelengths corresponds, respectively, to the third and fourth harmonics of the laser fundamental frequency. Pulses centered at 260 nm with excellent spatial profile, energies on the order of microjoules and temporal durations down to 18 fs, trough the compression by a prism pair, were obtained, which have wide applicability in nonlinear and time resolved optical spectroscopic studies. Ultrashort pulses at 195 nm where also obtained. An investigation of the influence of the spectral phase modulation of the laser pulses at 780 nm on the four-wave mixing nonlinear process for harmonic generation was also performed. In this way, a femtosecond pulse shaper based on a liquid crystal spatial light modulator in the 4f configuration was implemented in order to modulate the spectral phase of femtosecond pulses at 780 nm. This pulse shaper was then integrated to the system for generation of ultrashort pulses in the deep ultraviolet through the wave mixing process already implemented. This study aimed to obtain the indirect modulation of the 260 nm pulses spectral phase through the transfer of modulated spectral phase from pulses at 780 nm. Interesting initial results were obtained using a -step spectral phase, indicating the correct implementation of the system. The achievement of femtosecond pulses with modulated spectral phase in the deep ultraviolet is of great interest to perform coherent control studies in this spectral range and also for basic studies of how the spectral phase transfer occurs with different nonlinear optical laser processes. High-harmonic generation experiments based in the phase-matched frequency conversion in noble gas filled hollow fiber technique, using femtosecond pulses at 400 nm and 800 nm, were carried out during a internship at University of Colorado, USA. In this study, using pulses at 400 nm, an increase higher than one order of magnitude was obtained in the spectral region of 60 eV compared to harmonics generated, in this same region, with pulses at 800 nm. Finally, through the experience obtained during this internship, were carried out in our laboratory the development and implementation of a high harmonic generation system, based on the frequency conversion in a hollow fiber filled with argon gas. High harmonics with energies around 40eV (31nm) were obtained, and the conversion under phase-matched condition was demonstrated. Using pulses centered at 780nm, the highest harmonic order measured was 27 (28.9nm, 42.9eV), due to the spectral range limitation of monochromator used in our experiments. With the implementation of this system, becomes available at the Photonics Group a coherent light source at extreme ultraviolet wavelengths, which the unique properties have been already widely explored on a diversity of fundamental studies in basic and applied science.

Dans cette thèse, on s’intéresse à l'étude théorique et à la simulation numérique de la dynamique de charges et de spins dans des nano-structures métalliques. Ces dernières années la physique des nano-structures métalliques à connu un intérêt croissant, aussi bien d'un point de vue de la physique fondamental que d'un point de vue des applications technologiques. Il est donc essentiel d'avoir des modèles théoriques nous permettant de décrire correctement ce type d'objets. Cette thèse comporte deux études distinctes. Dans un premier temps on utilise un modèle semi-classique dans l'espace des phases afin d'étudier la dynamique de charges et de spins dans des films ferromagnétiques(Nickel). On décrit dans le même modèle le magnétisme itinérant et le magnétisme localisé. On montre qu'il est possible, en excitant le système avec un laser pulsé femtoseconde dans le domaine du visible, de créer un courant de spin oscillant dans la direction normal du film sur des temps ultrarapides(femtoseconde). Dans un second temps on s’intéresse à la dynamique de charge d'électrons confinés dans des nano-particules d'Or ou bien encore par des potentiels anisotropes. On montre que de telles systèmes sont des candidats intéressant pour faire de la génération d'harmoniques. / In this thesis we focus on the theoritical description and on the numerical simulation of the charge and spin dynamics in metallic nano-structures. The physics of metallic nano-structures has stimulated a huge amount of scientific interest in the last two decades, both for fundamental research and for potential technological applications. The thesis is divided in two parts. In the first part we use a semiclassical phase-space model to study the ultrafast charge and spin dynamics in thin ferromagnetic films (Nickel). Both itinerant and localized magnetism are taken into account. It is shown that an oscillating spin current can be generated in the film via the application of a femtosecond laser pulse in the visible range. In the second part we focus on the charge dynamics of electrons confined in metallic nano-particles (Gold) or anisotropic wells. We show that such systems can be used for high harmonic generation.

The multiconfiguration time-dependent Hartree-Fock (MCTDHF) and multiconfiguration time-dependent Hartree (MCTDH) methods are employed to investigate nonperturbative multielectron dynamics in finite quantum systems. MCTDHF is a powerful tool that allows for the investigation of multielectron dynamics in strongly perturbed quantum systems. We have developed an MCTDHF code that is capable of treating problems involving three dimensional (3D) atoms and molecules exposed to strong laser fields. This code will allow for the theoretical treatment of multielectron phenomena in attosecond science that were previously inaccessible. These problems include complex ionization processes in pump-probe experiments on noble gas atoms, the nonlinear effects that have been observed in Ne atoms in the presence of an x-ray free-electron laser (XFEL) and the molecular rearrangement of cations after ionization. An implementation of MCTDH that is optimized for two electrons, each moving in two dimensions (2D), is also presented. This implementation of MCTDH allows for the efficient treatment of 2D spin-free systems involving two electrons; however, it does not scale well to 3D or to systems containing more that two electrons. Both MCTDHF and MCTDH were used to treat 2D problems in nanophysics and attosecond science. MCTDHF is used to investigate plasmon dynamics and the quantum breathing mode for several electrons in finite lateral quantum dots. MCTDHF is also used to study the effects of manipulating the potential of a double lateral quantum dot containing two electrons; applications to quantum computing are discussed. MCTDH is used to examine a diatomic model molecular system exposed to a strong laser field; nonsequential double ionization and high harmonic generation are studied and new processes identified and explained. An implementation of MCTDHF is developed for nonuniform tensor product grids; this will allow for the full 3D implementation of MCTDHF and will provide a means to investigate a wide variety of problems that cannot be currently treated by any other method. Finally, the time it takes for an electron to tunnel from a bound state is investigated; a definition of the tunnel time is established and the Keldysh time is connected to the wavefunction dynamics.

La génération d’harmoniques d’ordre élevé est un processus d’interaction lumière-matière hautement non-linéaire permettant la synthèse d’impulsions sub-femtosecondes, dites attosecondes (1 as = 10⁻¹⁸ s). Mes travaux de thèse portent sur l’étude du transfert de moment angulaire lors de ce processus, afin de contrôler les caractéristiques spatiales et de polarisation du rayonnement émis dans l’extrême ultraviolet. Comme pour la matière, le moment angulaire de la lumière peut être séparé en une composante de spin, associée à l’état de polarisation du faisceau, et une composante orbitale, reliée à la forme du front d’onde. La maitrise complète du moment angulaire des harmoniques nécessite de recourir à des schémas de génération à deux faisceaux non-colinéaires, créant un réseau de diffraction dans le milieu générateur. Nous avons montré que, bien que les règles de transfert obéissent à des lois de conservation du moment angulaire, la description fine du phénomène requiert une analyse précise du champ laser dans le milieu de génération. Ces travaux ouvrent des perspectives de mise en forme avancée des impulsions attosecondes. / High-order harmonic generation is a highly nonlinear laser-matter interaction process which allows the synthesis of sub-femtosecond pulses, also called attosecond (1 as = 10⁻¹⁸ s) pulses. My PhD is centered around the study of angular momentum transfer during this process, in order to control spatial and polarization features of the radiation which is emitted in the extreme ultraviolet. As for matter, the angular momentum of light can be divided into a spin component, associated with the beam’s polarization, and an orbital component, related to the shape of the wavefront. The control of high harmonics’ angular momentum requires generating schemes involving two crossing beams, thus creating a diffraction grating in the generating medium.We have shown that, although the transfer rules obey conservation laws of the angular momentum, the fine description of the phenomenon requires an accurate analysis of the laser field in the generation medium. This work opens the road for advanced shaping of attosecond pulses.

Les impulsions ultra-brèves de rayonnement ultraviolet extrême (UVX) ont un grand champ d’application dans les domaines tels que le diagnostic de plasmas, la spectroscopie ou l’étude de la dynamique ultrarapide dans les atomes et les molécules.Aujourd’hui, il existe trois sources délivrant ce genre d’impulsions. Les harmoniques d’ordre élevé (HHG, en anglais) générés dans les gaz rares ou sur les solides peuvent fournir des impulsions attosecondes. Cependant, leur énergie, le plus souvent de l’ordre du nanojoule, limite les applications. L’amplification des impulsions harmoniques dans les plasmas créés par laser (SXRL, en anglais) a démontré pouvoir fournir des énergies de plusieurs dizaines de microjoules. Des énergies plus élevées peuvent être obtenues avec les lasers à électrons libres (LEL) UVX injectés, mais ce sont des Très Grandes Infrastructures ayant un accès limité.Ces dernières années, des progrès significatifs ont été réalisé avec chacune des ces sources, avec pour objectif la génération d’impulsions plus brèves. Il est devenu nécessaire de développer des nouvelles techniques de métrologie temporelle des impulsions UVX ultra-brèves. De plus, beaucoup d’expériences, comme ceux impliquant des phénomènes non-linéaires, nécessitent de hautes intensités UVX. La focalisation efficace des impulsions de faibles énergies peut significativement augmenter le domaine d’application. De bons fronts d’onde sont nécessaires pour focaliser les impulsions UVX à haute intensité, et les optiques doivent aussi être de bonne qualité et alignées avec précision.Dans cette thèse, les propriétés spatiales des harmoniques d’ordre élevé ont été extensivement étudiées grâce à un senseur de front d’onde UVX. Cet appareil couplé à une source HHG a démontré être utile pour la caractérisation de table et à la longueur d’onde ainsi que pour l’optimisation de systèmes optiques UVX.Le problème de la mise en place de la complète caractérisation temporelle d’impulsions UVX est aussi discuté en détail, et deux nouveaux schémas pour la reconstruction d’impulsions de LEL injectés et de lasers X à plasma sont présentés. Finalement, la première implantation d’un système d’amplification à dérive de fréquence (CPA, en anglais) sur un LEL UVX est présentée et son implantation pour les lasers X à plasmas est aussi discutée. / Ultrashort pulses of extreme-ultraviolet (XUV) radiation have a wide range of applications in fields such as plasma probing, spectroscopy, or the study of ultrafast dynamics in atoms and molecules.Nowadays, there are three main sources of such pulses. High-order harmonic generation (HHG) in rare gases or solid surfaces is able to provide attosecond pulses. However, their limited energy, of the order of nanojoules, limits its number of applications. The amplification of high-harmonic pulses in laser-driven plasmas (SXRL) has been demonstrated to provide energies of tens of microjules. Higher pulse energies can be obtained from seeded XUV free-electron lasers (FELs), large-scale facilities with more limited accessibility.In recent years, significant progress has been made with each of these sources towards the generation of shorter pulses. It is thus necessary to develop new techniques for full temporal metrology of ultrashort XUV pulses. Additionally, many experiments, such as those involving nonlinear phenomena, require high XUV intensities. Efficient focusing of low-energy pulses can significantly increase their range of application. Good wavefronts are required in order to focus XUV pulses to high intensities, and the optics must be of high quality and precisely aligned.In this thesis, the spatial properties of high-harmonic pulses are extensively explored thanks to the use of an XUV Hartmann wavefront sensor. This device is also proven here to be useful for tabletop, at-wavelength characterization and optimization of XUV optical systems with HHG sources.The problem of performing full temporal characterization of XUV pulses is also discussed in detail, and two new schemes for complete pulse reconstruction for seeded XUV FELs and seeded SXRLs are presented. Finally, the first implementation of chirped pulse amplification (CPA) in a seeded XUV FEL is reported, and its implementation in seeded SXRLs is discussed as well.

Cette thèse fait l'étude expérimentale de dynamiques de relaxations ultrarapides au sein d'atomes et de molécules (Ar, NO2, C2H2). Les méthodes expérimentales qui sont utilisées sont basées sur l'interaction d'un rayonnement laser avec le système atomique ou moléculaire étudié et font intervenir le processus de génération d'harmoniques d'ordres élevés, ainsi que la spectrométrie d'imagerie de vecteur vitesse. Au cours de cette thèse, deux approchesexpérimentales de type pompe-sonde ont été mises en œuvre. Une première approche exploitela sensibilité du processus de génération d'harmoniques à la structure électronique dumilieu pour la sonder. Cette méthode a été utilisée sur la molécule de dioxyde d'azote pourobserver sa relaxation électronique à travers l'intersection conique des états X2A1-A2B2suite à une excitation autour de 400 nm. Une seconde approche utilise le rayonnementharmonique comme source de photons dans le domaine de l'extrême ultraviolet (EUV)pour exciter ou sonder les espèces d'intérêt. Cette approche a été couplée avec l'utilisationd'un spectromètre d'imagerie de vecteur vitesse (VMIS), qui a été développé durant lathèse. Des expériences menées sur un système modèle comme l'argon ont permis de validerle dispositif expérimental, qui a ensuite été mis en application pour étudier la photodissociationde la molécule d'acétylène, après excitation autour de 9,3 eV du complexe deRydberg 3d-4s. Les deux méthodes mises en œuvre permettent toutes-deux de réaliserdes études dynamiques résolues en temps à l'échelle femtoseconde. / Ultrafast atomic and molecular dynamics (Ar, NO2, C2H2) have been experimentally studied during this PhD. The employed techniques use the laser interaction with the atomic or molecular system produced in gas phase. High harmonic generation (HHG) pump-probe studies allow resolving dynamics on a femtosecond scale. Two applications of high harmonic generation have been implemented here. In the first one, the harmonic generation process is the probe of a vibronic relaxation induced by a pump pulse. This application is currently labeled high harmonic spectroscopy. The sensibility of the high harmonic process to the geometry of the atomic or molecular orbitals is exploited to obtain information about the electronic structure of the generating medium. This method have been used to reveal the electronic relaxation of the nitrogen dioxide molecule (NO2) through the X2A1-A2B2 conical intersection.A second way consists to use the harmonic radiation like a source of XUV photons. The produced XUV radiation permits thus to reach electronically excited energy levels of atoms or molecules, pumping only with a one photon transition. XUV photons can also be used like a probe to ionize products of a molecular reaction. Velocity map imaging spectrometer (VMIS) have been designed and built to complete this fs-VUV source. Above threshold ionization (ATI) experiments and pump-probe XUV-400 nm studies have been performed on reference system like Argon to characterize the built experimental setup. The last excitation scheme has been also applied to study the photodissociation of the Acetylene excited in the 3d-4s Rydberg complex.

No description available.

Grâce à ses propriétés (cohérence, brillance, durée), le rayonnement XUV femtoseconde produit par génération d'harmoniques d'ordre élevé est utilisé comme un processus de sonde pour l'étude de dynamiques atomiques et moléculaires, avec une bonne résolution spatiale et temporelle (femtoseconde voire attoseconde). Ainsi, des dynamiques rotationnelles ont été résolues sur des petits systèmes moléculaires (N2, CO2). Les travaux de cette thèse ont consisté à étendre les méthodes de spectroscopie harmoniques et les appliquer à des systèmes moléculaires complexes d'intérêt femtochimique. Parmi elles, nous présenterons la génération d'harmoniques à deux sources, le réseau transitoire d'excitation ou encore la génération d'harmoniques à deux couleurs. Ces techniques nous ont permis de résoudre des dynamiques femtosecondes dans N2O4 et SF6. La HHG est aussi utilisée comme source de rayonnement XUV, en jouant le rôle d'impulsion pompe lors d'expériences de type pompe-sonde. Cette approche a été utilisée pour l'étude du dichroïsme circulaire de photoélectrons de molécules chirales ionisées par un champ XUV harmonique de polarisation quasi circulaire. Nous nous attarderons à détailler la découverte de cette nouvelle source XUV femtoseconde de polarisation quasi circulaire. / High harmonic generation (HHG) spectroscopy has proven to be a promisingtool (like probe in pump-probe experiments) in revealing the atomic and molecular dynamicswith the potential for subangstrom spatial resolution and subfemtosecond temporalresolution. Then, rotational dynamics have been resolved on small molecular systems (N2,CO2). This thesis looks to extending HHG spectroscopy methods to probe the structureand the dynamic of complex molecular systems. We will describe the two sources highharmonic generation, the transient grating of excitation and the two-color high harmonicgeneration. We enable to resolve the femtosecond nuclear dynamics in N2O4 and SF6. HHGis also used like a XUV radiation source, playing the role of pump pulse. This approach hasbeen used for the study of photoelectron circular dichroism. An XUV harmonic field witha quasi-circular polarization ionizes chiral molecules. In this manuscript, we will developthis new femtosecond XUV and quasi circular polarization radiation.