In the field of second harmonic (SH) generation most studies have been concerned with maximizing conversion efficiencies, generally achievable at the phase matching (PM) condition. Outside of the PM the conversion efficiency drastically decreases. This has caused that the possible working conditions out of PM to remain largely unexplored. In this thesis work we initiated a systematic study of the SH behavior in under conditions of large phase mismatch. When a pump pulse crosses an interface between a linear and a nonlinear medium there are always two generated SH components. These components may be understood on the basis of the mathematical solution of the inhomogeneous wave equations at the SH frequency. The homogeneous (HOM) solution is a component with wave-vector k(2¿) as expected from the dispersion relation and exchanges energy with the pump until the inevitable walk-off. The inhomogeneous (INH) solution is a component with a wave-vector 2k(¿), twice the pump wave-vector, and travels locked to the pump pulse. We divide our work in two parts, one for each generated component. Inhomogeneous component. We start a systematic study of the behavior of the generated INH component, phase locked to the pump. The consequences of phase locking (PL) can guide us towards new scenarios by allowing working conditions hitherto assumed inaccessible for absorbing materials. We show that while the HOM component travels with the group velocity given by material dispersion, the IHN component is captured by the pump pulse and experiences the same effective dispersion of the pump. It does not follow the PM condition. It naturally follows that the suppression of absorption at the SH wavelengths will occur if the pump is tuned to a region of transparency. We extended the same theory for the generated third harmonic (TH). We then studied the surprising behavior of SH and TH INH components with frequencies above the absorption edge when the material is placed inside a cavity resonant only at the fundamental frequency. We have shown that the PL mechanism not only inhibits absorption but also fosters the enhancement of harmonic generation by several orders of magnitude compared to the no-cavity case. Finally, we tested the INH SH and TH behaviors in metallic frequency regime of material. Homogeneous component. The techniques used to PM the nonlinear interaction enable efficient nonlinear interactions but drastically limit the spectral bandwidth of the nonlinear optical process, making the designed frequency converter only suitable for a fixed input wavelength and single interaction only. It has been shown that the use of disordered nonlinear media relaxes the PM condition thus allowing one to achieve relatively efficient broad bandwidth regime of the frequency conversion. An example of a quadratic nonlinear medium with a disordered domain structure is an un-poled Strontium Barium Niobate (SBN) crystal. It is composed of a system of random size anti parallel ferroelectric domains that allow to phase-match any second-order parametric process over a broad range of wavelengths without any poling. We have initiated an experimental and theoretical investigation of the properties of the SH waves generated in SBN crystals, with an extension to the generated TH. This study covers the coherence and polarization properties of the generated signal, as well as its spatial distribution. In addition, we have made an experimental study of the noncollinear interaction of short optical pulses in a SBN crystal by using two fundamental waves intersecting inside the crystal. We have shown that this effect may be employed as a simple tool for monitoring both the pulse duration and initial chirp. This method offers a simple and economic alternative to the existing methods for pulse characterization.

Lesões dentais por erosão têm sido cada vez mais presentes na prática clínica. A restauração direta com resina composta é uma das opções de tratamento para lesões severas, em que há comprometimento estético/funcional. Com o aprimoramento da tecnologia, a utilização do laser para pré-tratamento da superfície dentinária, antes do condicionamento ácido, tem sido considerada como método alternativo para melhorar a adesão das resinas compostas às superfícies erodidas. Assim, o objetivo deste estudo in vitro foi avaliar a influência da irradiação com laser de Er:YAG (2,94 ?m), de pulso super-curto, na adesão da resina composta à superfície dentinária erodida. Quarenta e seis discos de dentina foram obtidos a partir de 46 dentes terceiros molares humanos. A dentina oclusal planificada de 40 molares humanos teve metade de sua face protegida com fita UPVC (dentina hígida), enquanto na outra metade foi produzida uma lesão de erosão através da ciclagem em ácido cítrico (0,05 M, pH 2,3, 10 minutos, 6x/dia) e solução supersaturada (pH 7,0, 60 minutos entre os ataques ácidos). Metade das amostras foi irradiada com o laser de Er:YAG (50 ?s, 2 Hz, 80 mJ, 12,6 J/cm2) e a outra não (grupo controle). Em cada grupo de tratamento (laser ou controle) (n=10), um sistema adesivo autocondicionante foi utilizado e, então, confeccionados 2 cilindros de resina composta, tanto do lado erodido como no hígido (total de 4 cilindros), os quais foram submetidos à avaliação da Resistência de União através do ensaio de microcisalhamento (1 mm/min), após armazenamento em saliva artificial por 24 h. A análise do padrão de fratura foi realizada em microscópio óptico (40x). Por meio da Microscopia Eletrônica de Varredura (MEV), a morfologia das superfícies dentinárias hígida e submetida ao desafio erosivo, antes e após o tratamento com laser de Er:YAG (n=3), foi avaliada. Os valores obtidos de resistência de união (MPa) foram submetidos ao teste ANOVA e de comparações múltiplas de Tukey (p<0,05) e as análises das eletromicrografias foram feitas de forma descritiva. A análise morfológica da superfície mostrou alterações significativas na dentina hígida irradiada e na submetida à ciclagem erosiva, irradiada ou não. Quanto à resistência de união, houve diferença entre os 4 substratos analisados, sendo: dentina hígida irradiada (12,77±5,09 A), dentina hígida não irradiada (9,76±3,39 B), dentina erodida irradiada (7,62±3,39 C) e dentina erodida não irradiada (5,12±1,72 D). Houve predominância de padrão de fratura do tipo adesiva. Com base nos resultados e nos parâmetros de irradiação utilizados neste estudo, pode-se concluir que a erosão reduz a adesão em dentina e que o tratamento da superfície dentinária com laser de Er:YAG de largura de pulso super curta aumenta a adesão no substrato erodido ou hígido. / Dental erosion injuries have been increasingly present in clinical practice. Direct restoration with composite resin is one of the treatment options for severe injuries, where there is aesthetic/functional impairment. With the improvement of technology, laser-irradiation for pre-treatment of dentin before surface etching has been considered as an alternative method to improve the adhesion of composite resins to eroded surfaces. The objective of this in vitro study was to evaluate the influence of the irradiation with a super-short pulse Er:YAG (2.94 ?m) laser to the adhesion of composite resin to eroded dentin surface. Forty six dentin discs were obtained from 46 third molars. Forty samples of planned occlusal dentine, obtained from human molars, had half of their surface protected with plastic tape (sound dentin), while the other half was submitted to erosive cycles, consisted on immersion on citric acid (0.05 M, pH 2.3, 10 minutes, 6x/day) and supersaturated solution (pH 7.0, 60 minutes of acid attacks). Half of the samples was irradiated with the Er:YAG laser (50 ?s, 2 Hz, 80 mJ, 12.6 J/cm2) and the other was kept as control. In each treatment group (n = 10), a self-etching adhesive system was used and then two cylinders of composite resin were prepared, on both eroded and sound dentin (total of 4 cylinders). Microshear bond strength test was performed (1 mm/min), after 24 hours storage in artificial saliva. The analysis of the fracture pattern was determined by optical microscopy (40x). The morphology of sound and eroded dentin, before and after treatment with the Er:YAG laser (n = 3) was evaluated under Scanning Electron Microscopy (SEM). Bond strength values (MPa) were subjected to ANOVA and Tukey multiple comparisons test (p<0.05). The analyses of electron micrographs were made descriptively. Morphological analysis of the surface showed significant changes in irradiated and sound dentin subjected to erosive cycling. As for the bond strength, there were differences among the groups, as follows: sound dentin submitted to irradiation (12.77 ± 5.09 A), non-irradiated sound dentin (9.76 ± 3.39 B), eroded dentin submitted to irradiation (7 62 ± 3.39 C) and non-irradiated eroded dentin (5.12 ± 1.72 D). There was a predominance for the adhesive mode of failure. It was concluded that the erosion reduces the adhesion to dentin and that treating the dentin surface with a super-short-pulse Er:YAG laser increases adhesion to both eroded or sound dentin.

Au cours de dix dernières années la science aux attoseconde ou Physique au champ-fort a été l’objet d’un fort développement. La production d’impulsions laser énergétiques de courte durée à haute cadence et stabilisées en CEP constitue la première étape pour accéder aux dynamiques ultra-rapides caractérisant l’interaction de la matière avec une source de lumière cohérente, intense et ultra-rapide. Le travail de cette thèse consiste à améliorer globalement les performances d’un système laser Ti:Sa à haute cadence optimisé pour la génération des impulsions attoseconde. Nous avons développé une nouvelle configuration de cavité régénérative fonctionnant à 10 kHz qui permet une meilleure gestion des effets thermiques dans le cristal. En sortie de l’amplificateur les impulsions atteignent des valeurs de puissance de 5 W en bande étroite (35 fs), ou 2.7 W en bande spectrale large permettant une compression des impulsions proche de 17 fs. La CEP des impulsions en sortie d’amplificateur a été stabilisée ; le bruit résiduel mesuré tir-à-tir est de 210 mrad pendant trois heures.L’amplificateur peut supporter également le fonctionnement en mode accordable, en sélectionnant des spectres de 30 à 40 nm de largeur à mi-hauteur et en accordant leur longueur d’onde centrale dans une gamme de 80 nm autour de 800 nm. Nous avons conçu et mis en fonctionnement un amplificateur multi-passages non-cryogéné à imagerie par lentille thermique pour accroître la puissance des impulsions jusqu’à 10 W à une cadence de 1 kHz. Le régime de forte saturation d’amplificateur garantit une variation négligeable (±3% pic à pic) de la puissance des impulsions en sortie du module, face à une variation importante de la puissance en entrée (±25% pic à pic) sur la bande spectrale accordable. L’amplification peut encore être plus importante grâce à une ligne d’amplification à refroidissement cryogénique, qui permet d’atteindre des puissances au niveau TW, à la cadence de 1 kHz, tout en maintenant un régime de courte durée (17.5 fs) et stabilité en CEP (350 mrad de bruit résiduel tir-à-tir). Nous proposons aussi une étude des sources de bruit de CEP dans les modules hautement dispersifs: nous avons conçu une nouvelle approche numérique sur la base d’un logiciel de tracé de rayon commercial (Zemax) pour évaluer les variations de CEP dans les modules contenant réseaux de diffraction. / The last decade has seen a lot of progress in attosecond science or in strong field physics. Generating energetic, few-cycle laser pulses with stabilized Carrier-Envelope Phase at high repetition rate constitutes the first step to access the ultra-fast dynamics underlying the interaction of matter with intense, ultrashort coherent light source. The work of this thesis consists in globally improving the performances of a high repetition rate Ti:Sa laser system optimized for attosecond science. We present an original 10 kHz Ti:Sa CPA laser based on an newlydesigneddouble-crystal cavity for thermal lensing management. The amplifier delivers up to 5 W in narrow band mode (35 fs pulses), or 2.7 W in broad band mode, supporting 17 fs pulses after temporal compression. We demonstrate shot-to-shot CEP stabilization with a remaining noise of 210 mrad over three hours at the front-end output. In parallel to the short pulse duration operation mode, it is possible to use the front end in a wavelength tunability mode within a 80 nm range around 800 nm, with a resolution of 1 nm and 30 to 40 nm of bandwidth. We designed and demonstrated a complete water-cooled lens-less multipass amplifier using thermal lensing for modeadaptation boosting the pulse energy up to 10mJ at 1 kHz repetition rate (up to 10 W). The saturation regime of the amplifier ensures negligible variation (±3% peak to peak) of the output power for significant variation of the input power (±25% peak to peak) over the tunability range. The energy scalability of the front-end is demonstrated by coupling its output to cryogenically cooled amplifier, delivering 1 kHz, TW-class pulses at 17.5 fs and CEP stabilized with a residual noise of 350 mrad. A study of CEP noise sources in high dispersive module is also addressed, proposing a numerical approach based on a commercial ray-tracing software (Zemax) for predicting CEP fluctuation in grating based modules.

Master of Science / Department of Physics / Brian R. Washburn / This thesis reports our attempt towards achieving a phase stabilized free-space nonlinear polarization rotation (NPR) mode locked erbium doped fiber laser frequency comb system. Optical frequency combs generated by mode-locked femtosecond fiber lasers are vital tools for ultra-precision frequency metrology and molecular spectroscopy. However, the comb bandwidth and average output power become the two main limiting elements in the application of femtosecond optical frequency combs. We have specifically investigated the free-space mode locking dynamics of erbium-doped fiber (EDF) mode-locked ultrafast lasers via nonlinear polarization rotation (NPR) in the normal dispersion regime. To do so, we built a passively mode-locked fiber laser based on NPR with a repetition rate of 89 MHz producing an octave-spanning spectrum due to supercontinuum (SC) generation in highly nonlinear fiber (HNLF). Most significantly, we have achieved highly stable self-starting NPR mode-locked femtosecond fiber laser based frequency comb which has been running mode locked for the past one year without any need to redo the mode locking. By using the free-space NPR comb scheme, we have not only shortened the cavity length, but also have obtained 5 to 10 times higher output power (more than 30 mW at central wavelength of 1570 nm) and much broader spectral comb bandwidth (about 54 nm) compared to conventional all-fiber cavity structure with less than 1 mW average output power and only 10 nm spectral bandwidth. The pulse output from the NPR comb is amplified through a 1 m long EDF, then compressed by a length of anomalous dispersion fiber to a near transform limited pulse duration. The amplified transform limited pulse, with an average power of 180 mW and pulse duration of 70 fs, is used to generate a supercontinuum of 140 mW. SC generation via propagation in HNLF is optimized for specific polling period and heating temperature of PPLN crystal for SHG around 1030 nm. At last, we will also discuss the attempt of second harmonic generation (SHG) by quasi phase matching in the periodically polled lithium niobate (PPLN) crystal due to nonlinear effect corresponding to different polling period and heating temperature.

This thesis is concerned with various methods for the control and investigation of pulse dynamics in a Photonic Crystal Fibre (PCF) and of the radiation driven by a short pulse. In particular the focus is on pulses in the anomalous dispersion region which would form solitons in the absence of higher order effects. Several different types of radiation can be driven by such pulses if they are perturbed by higher order dispersive and non-linear effects - for example Resonant Radiation (RR) and Negative Resonant Radiation (NRR) two dispersive waves which gain energy at the expense of the pulse. The feature of NRR which is of particular importance is that it is the first observed example of a coupling between positive and negative frequencies in optics. This has only been possible due to recent advances in fields such as PCFs, lasers and analogue systems. As with many scientific discoveries, NRR was found by bringing together ideas and techniques from these different fields. Both the pulse and the driven radiation are investigated using a number of different pulse and PCF parameters. These include power, chirp, polarisation and PCF dispersion. These are used to vary the wavelengths at which the driven radiation occurs as well as its generation efficiency. Furthermore the power and chirp are used to vary where in the PCF the driven radiation is generated by controlling where the driving pulse compresses and spectrally expands. This property is used to investigate different stages in the evolution of the pulse and driven radiation as well as to optimise the generation efficiency of the driven radiation.

Das Ziel der vorliegenden Arbeit ist es, nanokristalline und laserpuls-strukturierte Elektroden für die alkalische Wasserelektrolyse zu untersuchten und hinsichtlich ihrer elektrokatalytischen Eigenschaft zu bewerten. Dabei besteht die Hauptaufgabe in der Aufklärung der Zusammenhänge zwischen der elektrokatalytischen Aktivität und der Struktur der Elektroden. Es soll der Effekt der nanokristallinen Kristallstruktur auf die Elektrodenaktivität aufgeklärt werden. Zudem stellt die elektrokatalytische Wirkung von Mo in Ni-Elektroden für die Wasserstoffentwicklungsreaktion eine zentrale Untersuchung in der vorliegenden Arbeit dar. Für die Sauerstoffentwicklungsreaktion soll der Einfluss von Fe in nanokristallinen Ni-Materialien näher analysiert und unter industriell relevanten Betriebsbedingungen bewertet werden. Zum anderen richtet sich der Fokus auf die Nutzung eines Ultrakurzpulslasers zur Strukturierung von Ni-Elektrodenoberflächen. Besonderes Augenmerk wird auf die Korrelation zwischen den individuellen Strukturmerkmalen, der erzielten Oberflächenvergrößerung und der elektrokatalytischen Aktivität bezüglich der Wasserstoffentwicklung gelegt. Zudem werden Langzeituntersuchungen bei Stromdichten von bis 1 A/cm² durchgeführt, um die Stabilität zu bewerten und Degradationsmechanismen aufzuklären.

Dans cette thèse, nous étudions expérimentalement la génération d'impulsions carrées très énergétiques et accordable à l’échelle nanosecondes et d'impulsions ultracourtes à haute puissance moyenne de sortie dans les lasers à fibre utilisant les nanomatériaux comme absorbant saturable. Tout d'abord, puisque la dynamique des impulsions est dominée par l'interaction de la non linéarité et de la dispersion chromatique cubique de la fibre avec un mécanisme de discrimination d'intensité appelé absorbant saturable, la stabilité d'une distribution harmonique en mode verrouillé est étudiée par injection externe d'une onde continue.Enfin, nous avons utilisés des absorbant saturable à base de nanomatériaux déposés sur des tapers optiques dans les lasers à fibre pour générer des impulsions ultracourtes avec une puissance de sortie moyenne élevée. / In this thesis, we investigate experimentally the generation of high energy nanosecond tunable square pulses and high output power ultrashort pulses in fiber lasers. First, since pulse dynamics are dominated by the interaction of the fiber's cubic Kerr nonlinearity and chromatic dispersion with an intensity-discriminating mechanism referred to as a saturable absorber, the stability of a harmonic mode-locked distribution is studied by external injection of a continuous wave. Finally, we implemented nanomaterial based saturable absorbers in fiber laser configuration to generate ultrashort pulses with high average output power. Different techniques of achieving such components are explicitly detailed: ultrashort pulse generation in ring cavities where graphene and topological insulators are deposited on optical tapers to form a saturable absorber.

In dieser Dissertation wird zum einen die ultraschnelle Ladungsträgerkinetik in einem Galliumnitrid (GaN)-basierten Übergitter, zum anderen die piezoelektrische Elektron-Phonon-Wechselwirkung kohärenter zonengefalteter Phononen in Galliumarsenid (GaAs)-basierten Übergittern behandelt. Mittels spektral- und zeitaufgelöster Photolumineszenzmessungen an einem n-dotierten GaN/Al0,18Ga0,82N Übergitter mit Parametern ähnlich derer in optoelektronischen Bauelementen wurde die defektbedingte Ladungsträgerkinetik untersucht, die innerhalb von ca. 150 ps durch den Einfang in tiefe, nichtstrahlende Rekombinationszentren beeinflusst wird. Die Untersuchung einer Passivierung mit Siliziumnitrid zur Verhinderung von Degradationseffekten zeigte ein stabiles optisches Langzeitverhalten bei gleichzeitiger Zunahme nichtstrahlender Defekte. Ferner wurde mit spektral aufgelöster Anrege-Abfrage-Spektroskopie eine Einfangkinetik auf einer Zeitskala von 150 - 200 fs in Defektzustände nahe der Übergitterbandkante gemessen, gefolgt von der Abkühlung der Ladungsträger durch Phononemission innerhalb weniger Pikosekunden bei Raumtemperatur und 35 ps bei 5 K. Kohärente zonengefaltete Phononen wurden mit Anrege-Abfrage-Spektroskopie an zwei AlAs/GaAs-Übergittern untersucht, die in [100]-, bzw. [111]-Richtung gewachsen wurden. Dies ermöglicht die (gezielte) Untersuchung der piezoelektrischen Elektron-Phonon-Kopplung, da diese für longitudinal-akustischen Phononen nur in der [111]-Probe existiert. Die Amplitude kohärenter Phononen mit einem Wellenvektor von q=0 in der [111]-Probe fällt verglichen mit denen in der [100]- und der [111]-Probe mit q≠0 signifikant schneller ab. Kohärente Phononen verursachen in der [111]-Probe bei q=0 ein makroskopisches piezoelektrisches Feld, welches Ladungsträger beschleunigt, die durch Reibung kohärente Phononen dämpfen. Bei hohen Ladungsträgerdichten unterdrückt die Abschirmung der induzierten piezoelektrischen Felder diese zusätzliche Dämpfung. / In this dissertation, the ultrafast carrier dynamics in a gallium nitride (GaN)-based superlattice as well as the piezoelectric electron-phonon-coupling of coherent zone-folded phonons in gallium arsenide (GaAs)-based superlattices are addressed. Using spectrally and time-resolved photoluminescence experiments on an exemplary n-doped GaN/Al0.18Ga0.82N superlattice with parameters similar to those in optoelectronic devices, we investigated the defect-related carrier kinetics, that are affected by trapping in saturable nonradiative recombination centers on time scales of ~150 ps. The investigation of a passivation with silicon nitride to prevent degradation effects show a long-term optical stability with a concomitant increase in non-radiative defect densities. Furthermore, spectrally resolved pump-probe spectroscopy was used to measure trapping kinetics into defect states near the conduction band minimum on a time scale of 150 – 200 fs. These kinetics are followed by carrier cooling through phonon emission within a few picoseconds at room temperature and within 35 ps at 5 K. Coherent zone-folded phonons were studied with pump-probe spectroscopy on two AlAs/GaAs superlattices grown in [100] and [111] direction, respectively. This allows the specific investigation of the piezoelectric electron-phonon interaction, since this exists for longitudinal acoustic phonons only in the [111] sample. The amplitude of coherent phonons with a wave vector of q=0 in the [111] sample decays significantly faster than in the [100] and the [111] samples with q≠0. Coherent phonons in the [111] sample cause a macroscopic piezoelectric field to which the photogenerated electron-hole plasma couples. Friction of the accelerated carriers provides the additional damping mechanism. High carrier densities screen the induced piezoelectric field, thus reducing the damping mechanism via the piezoelectric interaction.

La génération d'harmoniques d'ordre élevé en milieu gazeux est un phénomène habituellement décrit par un modèle à trois étapes : sous l'effet d'un champ laser intense, un atome (ou une molécule) est ionisé par effet tunnel. L'électron éjecté est accéléré dans le champ laser, puis il se recombine sur son ion parent en émettant un photon XUV. Ce rayonnement XUV, émis sous la forme d'impulsions attosecondes (1 as = 10-18 s), est un outil idéal pour sonder la structure électronique des atomes ou des molécules, avec une résolution temporelle de l'ordre de l'attoseconde. Néanmoins, l'intensité de ce rayonnement n'est en général pas suffisante pour induire des effets non-linéaires (transitions à deux photons).Au cours des travaux réalisés pendant cette thèse, nous avons développé une source harmonique capable de produire un rayonnement XUV intense qui doit permettre d'accéder à la physique non-linéaire dans cette gamme de longueur d'onde. Pour parvenir à ces résultats, un travail important sur les impulsions infrarouges génératrices a été nécessaire, aussi bien dans le domaine spatial que dans le domaine temporel. Une technique de mise en forme spatiale de faisceaux laser intenses a donc été développée, ainsi qu'une technique de post compression adaptée aux impulsions laser intenses. Ce travail de thèse se divise donc en trois étapes : - Le développement de la source harmonique haute énergie et des diagnostics associés. Cette source est basée sur l'utilisation d'une chaîne laser Titane-Saphir qui délivre des impulsions de 150 mJ pour des durées de 40 fs à une cadence de 10 Hz. De bonnes conditions d'optimisation ont été obtenues, donnant lieu à des impulsions XUV dont l'énergie est de l'ordre du µJ lors de la génération dans l'argon.- Le développement d'une technique de mise en forme spatiale adaptée aux faisceaux laser intenses et à la génération d'harmoniques. Le dispositif est basé sur une optique en réflexion et sur les interférences à deux faisceaux. Il permet de produire, dans la région focale, des faisceaux dont le profil d'intensité est radialement constant (faisceaux flat top) et ainsi d'apporter un contrôle supplémentaire sur la génération d'harmoniques d'ordre élevé.- Le développement d'une technique de post compression en propagation guidée basée sur l'élargissement spectral induit par ionisation. Cette technique est adaptée pour des impulsions intenses (3.5 TW) et permet de produire des impulsions de puissance crête supérieure au Térawatt dans le domaine sub-10 fs. Cette technique fournit donc une source unique pour la génération d'harmoniques d'ordre élevé.Ces deux approches ont été testées et validées pour la génération d'harmoniques d'ordre élevé, et les résultats obtenus ouvrent d'intéressantes perspectives telles que la génération d'impulsions attosecondes isolées de haute énergie (> 100 nJ). / The generation of high order harmonics in a gaseous medium is a phenomenon conveniently described by a three steps model : subject to a strong laser field irradiation, an atom (or molecule) can undergo a tunneling ionization. The ejected electron is accelerated in the laser field and recombine on its parent ion leading to the emission of an XUV photon. The XUV radiation can be emitted as attosecond pulses (1 as = 10-18 s), and it is then an ideal tool to probe the electronic structure of atoms or molecules which require the highest time resolution. However, the intensity of this radiation is usually not sufficient to induce non-linear processes (two-photon transitions).In the frame of this work, we have developed a harmonic source capable of producing an intense XUV radiation to access non-linear physics in this wavelength domain.To achieve these results, significant work on the infrared generating pulses was necessary, both in the spatial and temporal domain. We have developed a technique for spatial shaping of intense laser beams, and a post compression technique fitted to high energy pulses.This thesis is therefore divided into three parts:- The development of an high energy harmonic source and related diagnostics. We use a Ti: sapphire laser system for this source which delivers 40-fs pulses up to an energy of 150 mJ at 10 Hz repetition rate. Good optimization conditions were obtained, leading to XUV pulse energies of the order of μJ in the case of generation in argon.- The development of a spatial shaping technique adapted to intense laser beams and to harmonic generation. The device is based on reflection optics and the interferences of two beams. It can produce, in the focal region, beams with a radially constant intensity over a large volume (flat top beams) and thus provide additional control of the harmonics generating process.- The development of a post compression technique in guided geometry based on the ionization induced spectral broadening. This technique is suitable for intense pulses (3.5 TW) and produces pulses above the terawatt level in the 10-fs range. This technique therefore provides a unique source for harmonic generation.These two approaches have been tested and validated for high order harmonics generation, and the results open interesting perspectives such as the generation of isolated attosecond pulses of high energy (> 100 nJ).