The present thesis concerns aspects of the interaction ofmatter in gas, liquid and solid phases, with electromagneticradiation, ranging from the optical to the X-ray region. Overthe last decade the availability of ultrashort strong laserpulses as well as of high power synchrotron sources of tunableX-ray radiation has stimulated a rapid development of newexperimental techniques which makes it possible to analysedifferent physical, chemical and biological processes inunprecedented detail. All of this urges a concomitantdevelopment of adequate theoretical language and methodscombined with simulation techniques. The first part of the thesis addresses nonlinear propagationof strong optical pulses. This study is motivated by thebreakthrough in synthesis of novel organic materials possessingprespecified nonlinear optical properties and which has led toa multitude of potential applications such as, for example, 3Dimaging and data storage, optical limiting and photodynamiccancer therapy. In order to clarify the underlying physics, astrict solution has been derived of the density matrixequations of a material aiming at an explicit treatment of itsnonlinear polarization without addressing a conventional Taylorexpansion over field amplitudes. Such a formalism is developedfor many-level molecules, allowing to solve the coupledMaxwell's and density matrix equations for the propagation of afew interacting laser pulses through a nonlinear molecularmedium. The theory presented is capable to account formulti-photon processes of an arbitrary order and for differentsaturation effects. The theory is applied to simulations oftwo- and three-photon absorption as well as to upconvertedstimulated emission of organic molecules in solvents. The second part of the thesis is devoted to resonant X-rayRaman scattering from free molecules, solutions and polymerfilms. The temporal analysis of the spectral profiles isperformed using the technique of scattering duration whichallows to select physical processes with different time scales.The slowing-down/speeding-up of the scattering by frequencydetuning provides insight in the formation of the differentparts of the scattering profile like atomic and molecularbands, resonant and vertical scattering channels, anomalousenhancement of the Stokes doubling effect. The lifetimevibrational interference (LVI), playing a crucial role inresonant scattering, is found to strongly influence thedispersion of the Auger resonances of polymers in agreementwith experiment. An almost complete quenching of the scatteringcross section by LVI is observed for the N2molecule. It is found that the interferenceelimination of the scattering amplitude gives valuableinformation on molecular geometry. The electron Doppler effectis minutely studied making use of a wave packet technique. Thesimulations show an "interference burning" of a narrow hole onthe top of the Doppler broadened profile of the Auger spectraof molecular oxygen. For the SF6molecule the Auger Doppler effect is found to besensitive to the detuning due to the scattering anisotropy. Inall of these studies the temporal language was foundconstructive and enormously helpful for understanding theunderlying physical processes. Most theoretical predictionsmade have been verified by experiments.

<p>The present thesis concerns aspects of the interaction ofmatter in gas, liquid and solid phases, with electromagneticradiation, ranging from the optical to the X-ray region. Overthe last decade the availability of ultrashort strong laserpulses as well as of high power synchrotron sources of tunableX-ray radiation has stimulated a rapid development of newexperimental techniques which makes it possible to analysedifferent physical, chemical and biological processes inunprecedented detail. All of this urges a concomitantdevelopment of adequate theoretical language and methodscombined with simulation techniques.</p><p>The first part of the thesis addresses nonlinear propagationof strong optical pulses. This study is motivated by thebreakthrough in synthesis of novel organic materials possessingprespecified nonlinear optical properties and which has led toa multitude of potential applications such as, for example, 3Dimaging and data storage, optical limiting and photodynamiccancer therapy. In order to clarify the underlying physics, astrict solution has been derived of the density matrixequations of a material aiming at an explicit treatment of itsnonlinear polarization without addressing a conventional Taylorexpansion over field amplitudes. Such a formalism is developedfor many-level molecules, allowing to solve the coupledMaxwell's and density matrix equations for the propagation of afew interacting laser pulses through a nonlinear molecularmedium. The theory presented is capable to account formulti-photon processes of an arbitrary order and for differentsaturation effects. The theory is applied to simulations oftwo- and three-photon absorption as well as to upconvertedstimulated emission of organic molecules in solvents.</p><p>The second part of the thesis is devoted to resonant X-rayRaman scattering from free molecules, solutions and polymerfilms. The temporal analysis of the spectral profiles isperformed using the technique of scattering duration whichallows to select physical processes with different time scales.The slowing-down/speeding-up of the scattering by frequencydetuning provides insight in the formation of the differentparts of the scattering profile like atomic and molecularbands, resonant and vertical scattering channels, anomalousenhancement of the Stokes doubling effect. The lifetimevibrational interference (LVI), playing a crucial role inresonant scattering, is found to strongly influence thedispersion of the Auger resonances of polymers in agreementwith experiment. An almost complete quenching of the scatteringcross section by LVI is observed for the N₂molecule. It is found that the interferenceelimination of the scattering amplitude gives valuableinformation on molecular geometry. The electron Doppler effectis minutely studied making use of a wave packet technique. Thesimulations show an "interference burning" of a narrow hole onthe top of the Doppler broadened profile of the Auger spectraof molecular oxygen. For the SF₆molecule the Auger Doppler effect is found to besensitive to the detuning due to the scattering anisotropy. Inall of these studies the temporal language was foundconstructive and enormously helpful for understanding theunderlying physical processes. Most theoretical predictionsmade have been verified by experiments.</p>

No description available.

Ce manuscrit est consacré à la croissance par HVPE et à la spectroscopie optique de nanofils d'InxGa1-xN et de microfils de GaN en vue de la réalisation de diodes électroluminescentes. Les microfils de GaN, épitaxiés par SAG-HVPE, ont été étudiés par micro-réflectivité et micro-photoluminescence. Un lien entre les différences de polarités au sein des fils et leurs propriétés optiques a été mis en évidence. De plus, il a été démontré que les microfils agissent comme des résonateurs optiques dans lesquels une émission stimulée de lumière a été observée. Des reprises de croissance par MOCVD ont permis de révéler le potentiel des microfils pour la réalisation de DELs sous forme d'hétérostructures coeur - coquille. Les nanofils d'InxGa1-xN ont été obtenus pour la première fois à l'Institut Pascal grâce à une étude thermodynamique et une étude expérimentale utilisant GaCl et InCl3 comme précurseurs en éléments III. Une variation de composition en indium de 0 à 100 % le long d'un unique échantillon a été rapportée dans un premier temps. L'optimisation du positionnement des échantillons par rapport à l'arrivée du flux d'indium associée à une étude systématique de l’influence des différents paramètres de croissance a permis de déterminer les facteurs contrôlant la composition et la morphologie des fils. Une étude par spectroscopie optique en fonction de la température a finalement montré une faible diminution de l'intensité de photoluminescence entre 20 K et 300 K. / This work is devoted to the HVPE growth and to the optical spectroscopy of InxGa1-xN nanowires and GaN microwires in order to realize light-emitting diodes.The GaN microwires, grown by SAG-HVPE, were studied by micro-reflectivity and micro-photoluminescence. A link between the polarity differences within wires and their optical properties has been highlighted. In addition, microwires have been shown to act as optical resonators in which stimulated light emission has been observed. Regrowth by MOCVD revealed the potential of microwires for LEDs realization with a core - shell structure.The InxGa1-xN nanowires were obtained for the first time at Institut Pascal thanks to a both thermodynamical and experimental investigations using GaCl and InCl3 as III element precursors. An indium composition variation from 0 to 100 % along a single sample was first reported. The optimization of the sample positioning regarding the indium flux arrival associated with a systematic study of the influence of growth parameters have allowed to determine influential factors on the composition and the morphology of wires. A temperature dependent optical analysis has finally shown a slight decrease of luminescence intensity between 20 K and 300 K.

La filamentation laser femtoseconde dans l'air est un phénomène qui implique une riche famille d'effets optiques non linéaires. Effet laser de filaments a émergé comme un phénomène nouveau en 2011. Il a été activement étudiée au cours des dernières cinq années, non seulement en raison de ses applications potentielles dans les techniques de télédétection mais aussi la physique pour découvrir. Cette thèse est consacrée principalment à l'étude de deux types d'effets laser à partir du plasma filamentaire généré par 800 nm impulsions laser femtosecondes dans l'air ou l'azote pur. Le premier est l'émission spontanée amplifiée à 337 nm longueur d'ondes de molécules d'azote neutre qui est bidirectionnel, activée uniquement par des impulsions polarisées circulairement. Le mécanisme d'inversion de population est attribuée à électrons-molécules collisions inélastiques entre les électrons énergiques et les molécules d'azote neutres sur l'état du sol. La caractérisation complète de 337 nm impulsion laser vers l'avant et vers l'arrière est réalisée. En particulier, les mesures de profil temporelles sont comparées à des simulations numériques basées sur l'équation de Maxwell-Bloch à une dimension, qui se révèle être en bon accord. Un autre type d'effet laser est lié à ions d'azotes excités, émettant à 391 nm et 428 nm longueurs d'onde. Ce type d'effet laser est observée avec laser pompe polarisée linéairement. Il est caractérisé systématiquement dans des domaines spatiaux, temporels et spectrales. Les résultats du profil temporel prouve que l'émission laser ionique est fondamentalement superradiance. Un nouveau mécanisme, à savoir le processus d'excitation recollision d'électrons, est proposé pour la réalisation de la distribution de la population dans le niveau supérieur de la transition. Il est soutenu par deux mesures expérimentales consistant en la dépendance de 391 nm émission laser à l'ellipticité et la dépendance à longueur d'onde de laser pompe. Des simulations numériques donnent un bon accord avec l'observation expérimentale. / Femtosecond laser filamentation in air is a phenomenon that involves a rich family of nonlinear optic effects. Lasing effect from filaments has emerged as a new phenomenon in 2011. It has been actively studied in recent 5 years not only because of its potential applications in remote sensing techniques but also the fruitful physics involved. This thesis is devoted to the study of two types of lasing effect from filament plasma generated by 800 nm femtosecond laser pulses in air or pure nitrogen. The first is the bidirectional amplified spontaneous emission at 337 nm wavelength of neutral nitrogen molecules, only enabled by circularly-polarized pulses. The population inversion mechanism is attributed to inelastic electron-molecule collisions between energetic electrons and neutral nitrogen molecules on the ground state. Full characterization of both forward and backward 337 nm lasing pulse is conducted. Particularly the temporal profile measurements is compared to numerical simulations based on one-dimensional Maxwell-Bloch equation, which turns out to be in good agreement. Another type of lasing effect is related to excited nitrogen ion, emitting at 391 nm and 428 nm wavelengths. This type of lasing effect can only be observed with linearly-polarized pump laser. It is systematically characterized in spatial, temporal and spectral domains. The temporal profile results proves that ionic lasing emission is fundamentally superradiance. A new mechanism, namely the electron recollision excitation process, is proposed for the achievement of population distribution in the upper level of transition. It is supported by two experimental measurements consisting of pump ellipticity dependence and pump wavelength dependence of 391 nm lasing intensity. Numerical simulations give good agreement with the experimental observation.

No description available.

Organic microcavities comprising the host:guest emitter system Alq3:DCM offer an interesting playground to experimentally study the dispersion characteristics of laterally patterned microlasers due to the broad emission spectrum and large oscillator strength of the organic dye. By structuring of metallic or dielectric sublayers directly on top of the bottom mirror, we precisely manipulate the mode structure and in fluence the coherent emission properties of the device. Embedding silver layers into a microcavity leads to an interaction of the optical cavity-state in the organic layer and the neighboring metal which red-shifts the cavity resonance, creating a Tamm-plasmon-polariton state. A patterning of the metal can in turn be exploited to fabricate deep photonic wells of micron-size, efficiently confining light in lateral direction. In periodic arrays of silver wires, we create a Kronig-Penney-like optical potential in the cavity and in turn observe optical Bloch states spanning over several photonic wires. We modify the Kronig-Penney theory to analytically describe the full far-field emission dispersion of our cavities and show the emergence of either zero- , π-, or 2π- phase-locking in the system. By investigating periodic SiO2 patterns, we experimentally observe stimulated emission from the ground and different excited discrete states at room temperature and are able to directly control the laser emission from both extended and confined modes of the photonic wires at room-temperature.