Le progrès continu de la technologie laser a récemment permis l’avancement spectaculaire d’accélérateurs de particules par onde de sillage. Cette technique permet la génération de champs électriques très forts, pouvant dépasser de trois ordres de grandeurs ceux présents dans les accélérateurs conventionnels. L’accélération résultante a lieu sur une distance très courte, par conséquent les effets de la charge d’espace et de la dispersion de vitesse sont considérablement réduits. Les paquets de particules ainsi générés peuvent alors atteindre des durées de l’ordre de la femtoseconde, qui en fait un outil prometteur pour la réalisation d’expériences de diffraction ultra-rapide avec une résolution inégalée de l’ordre de quelques femtosecondes. La génération de tels paquets d’électrons avec des lasers de 1 J et d’une durée de 30 fs est à présent bien établie. Ces paramètres permettent de produire des faisceaux d’électrons de quelques centaines de MeV, et sont donc inadaptés aux expériences de diffraction. De plus, le taux de répétition de ces lasers de haute puissance est limité à quelques Hz, ce qui est insuffisant pour des expériences exigeant une bonne statistique de mesure. Notre groupe a utilisé un laser de pointe développé au laboratoire par le groupe PCO générant des impulsions de quelques millijoules, d’une durée de 3.4 fs - à peine 1.3 cycle optique - à une cadence de 1 kHz, pour accélérer des électrons par onde de sillage. Ce travail de thèse présente d’une part la première démonstration d’un accélérateur des particules relativistes opéré dans le régime de la bulle à haute cadence. L’utilisation de buses microscopiques a permis l’obtention de charges de dizaines de pC par tir. De plus, cette thèse vise à l’élargissement de notre compréhension des lois d’échelle d’accélération laser-plasma. Nous espérons que notre travail visant à la fiabilisation et l’optimisation de cette source permettra à terme de proposer un instrument accessible et fiable à la communauté scientifique, que ce soit pour la diffraction d’électrons, l’irradiation ultra-brève d’échantillons ou la génération de rayons X. / Continuing progress in laser technology has enabled dramatic advances in laser wakefield acceleration (LWFA), a technique that permits driving particles by electric fields three orders of magnitude higher than in conventional radio-frequency accelerators. Due to significantly reduced space charge and velocity dispersion effects, the resultant relativistic electron bunches have also been identified as a candidate tool to achieve unprecedented sub-10 fs temporal resolution in ultrafast electron diffraction (UED) experiments. High repetition rate operation is desirable to improve data collection statistics and thus washout shot-to-shot charge fluctuations inherent to plasma accelerators. It is well known that high-quality electron beams can be achieved in the blowout, or "bubble" regime, which is at present regularly accessed with ≈ 30 fs Joule-class lasers that can perform up to few shots per second. Our group on the contraryutilized a cutting edge laser system producing few-mJ pulses compressed nearly to a single optical cycle (3.4 fs) to demonstrate for the first time an MeV-grade particle accelerator with properties characteristic to the blowout regime operating at 1 kHz repetition rate. We further investigate the plasma density profile and exact laser pulse waveform effects on the source output, and show that using special gas microjets a charge of tens of pC/shot can be achieved. We expect this technique to lead to a generation of highly accessible and robust instruments for the scientific community to conduct UED experiments or to be used for other applications. This work also serves to expand our knowledge on the scalability of laser-plasma acceleration.

Lasers find a wide range of applications in many areas including photo-biology, photo-chemistry, materials processing, imaging and telecommunications. However, the practical use of such sources is often limited by the bulky nature of existing systems. By fabricating channel waveguides in solid-state laser-gain materials more compact laser systems can be designed and fabricated, providing user-friendly sources. Other advantages inherent in the use of waveguide gain media include the maintenance of high intensities over extended interaction lengths, reducing laser thresholds. This thesis presents the development of Yb:tungstate lasers operating around 1μm in waveguide geometries. An Yb:KY(WO₄)₂ planar waveguide laser grown by liquid phase epitaxy is demonstrated with output powers up to 190 mW and 76 % slope efficiency. This is similar to the performance from bulk lasers but in a very compact design. Excellent thresholds of only 40 mW absorbed pump power are realised. The propagation loss is found to be less than 0.1 dBcm⁻¹ and Q-switched operation is also demonstrated. Channel waveguides are fabricated in Yb:KGd(WO₄)₂ and Yb:KY(WO₄)₂ using ultrafast laser inscription. Several of these waveguides lase in compact monolithic cavities. A maximum output power of 18.6 mW is observed, with a propagation loss of ~2 dBcm⁻¹. By using a variety of writing conditions the optimum writing pulse energy is identified. Micro-spectroscopy experiments are performed to enable a fuller understanding of the induced crystal modification. Observations include frequency shifts of Raman lines which are attributed to densification of WO₂W bonds in the crystal. Yb:tungstate lasers can generate ultrashort pulses and some preliminary work is done to investigate the use of quantum dot devices as saturable absorbers. These are shown to have reduced saturation fluence compared to quantum well devices, making them particularly suitable for future integration with Yb:tungstate waveguides for the creation of ultrafast, compact and high repetition rate lasers.

This thesis considers the problem of calculating and observing the mixing of modes of positive and negative frequency in inhomogeneous, dispersive media. Scattering of vacuum modes of the electromagnetic field at a moving interface in the refractive index of a dielectric medium is discussed. Kinematics arguments are used to demonstrate that this interface may, in a regime of linear dispersion, act as the analogue of the event horizon of a black hole to modes of the field. Furthermore, a study of the dispersion of the dielectric shows that five distinct configurations of modes of the inhomogeneous medium at the interface exist as a function of frequency. Thus it is shown that the interface is simultaneously a black- and white-hole horizon-like and horizonless emitter. The role, and importance, of negative-frequency modes of the field in mode conversion at the horizon is established and yields a calculation of the spontaneous photonic flux at the interface. An algorithm to calculate the scattering of vacuum modes at the interface is introduced. Spectra of the photonic flux in the moving and laboratory frame, for all modes and all realisable increase in the refractive index at the interface are computed. As a result of the various mode configurations, the spectra are highly structured in intervals with black-hole, white-hole and no horizon. The spectra are dominated by a negative-frequency mode, which is the partner in any Hawking-type emission. An experiment in which an incoming positive-frequency wave is populated with photons is assembled to observe the transfer of energy to outgoing waves of positive and negative frequency at the horizon. The effect of mode conversion at the interface is clearly shown to be a feature of horizon physics. This is a classical version of the quantum experiment that aims at validating the mechanism of Hawking radiation.

Ein Ziel der Arbeit war die Entwicklung eines Verfahrens zur 3D-Positionierung auf Basis elektrooptischer Pseudostreckenmessung. Ein zweites Ziel war die Entwicklung eines Reflexgoniometers zur zweiachsigen Winkelmessung. Im Rahmen der Arbeit wurden die Grundlagen zur instrumentellen Umsetzung beider Verfahren erarbeitet, die Genauigkeitspotentiale ermittelt und mögliche Anwendungen für die einzelnen Schlüsseltechnologien und deren Kombination abgeleitet. In einer Prototyp-Entwicklung wurden Vorschläge für die wesentlichen Funktionselemente des räumlichen Weg- bzw. Winkelmesssystems gemacht. Hierzu gehören das kardanisch aufgehängte Etalon, die temperaturstabilisierte Laseroptik und die temperaturkalibrierte CCD der Winkelmesseinheit (Reflexgoniometer), die Systeme zur Erzeugung und Detektion ultrakurzer Laserpulse, eine elastische Optik, Möglichkeiten zur Formung des transversalen Strahlprofils, das TCSPC-System und die zur Auswertung und Kalibrierung notwendigen Algorithmen, wie z.B. die Autokollimation eines Lasers. ("Veröffentlicht von der Deutschen Geodätischen Kommission Reihe C (Dissertationen) unter der Nummer C 614 (München 2008; ISBN 3 7696 5053 0; 2; 144 S.") / One goal of the thesis was the development of a method for three-dimensional positioning based on electro-optical measurement of pseudo ranges. Another goal was the development of a reflex goniometer for biaxial angle measurement. Within the scope of this thesis the basics for the instrumental realisation of both methods were developed, the accuracy potentials were determined and possible applications for the separate key technologies and their combination were deduced. In a prototype development proposals were made for the main functional elements of the spatial distance and angle measurement systems. These include the gimbal mounted etalon, the temperature stabilised laser optics and the temperature calibrated CCD of the angle measurement device (reflex goniometer), the systems for creation and detection of ultrashort laser pulses, an elastic optical device, possibilities of transversal beam shaping, the TCSPC system and the algorithms which are necessary for analysis and calibration, e.g. the autocollimation of a laser.

A hybrid quantum-classical approach to the interaction of atomic clusters with intense laser fields in the vacuum ultra-violet (VUV) has been developed. Much emphasis is put on localized electrons, those quasi-free electrons which localize about the ions and screen them. These electrons set a time scale, which is used to interpolate between the quantum, rate based description of photon absorption by bound electrons and the classical, deterministic description of the cluster nano-plasma. Typical observables such as total energy absorption, electron and ion spectra are in very good agreement with the experimental findings. A scheme to probe the multi-electron motion in clusters with attosecond laser pulses is introduced. Conventional final state measurements in the energy domain cannot provide information about earlier states of the system due to the incoherent nature of the dynamics. Time-delayed attosecond pulses in the extreme ultra-violet (XUV) are used to probe the transient charging of the cluster ions during the interaction with the laser by measuring the kinetic energy of the electrons detached by the probe pulse. This information is otherwise lost at later times due to recombination. Knowledge about the transient charging would also shed more light on the still controversial subject of the energy absorption mechanisms in the VUV regime. Moving to shorter duration of the excitation, the characteristic time-scales for ionization and plasma equilibration are inversed. An attosecond laser pulse in the VUV regime creates a dense, warm nano-plasma far from equilibrium. Time-delayed attosecond pulses in the XUV probe then both the creation and the relaxation. The latter shows the breakup of the Bogoliubov hierarchy of characteristic times, indicating strongly-coupled plasma dynamics and drawing parallels to the relaxation of extended ultra-cold neutral plasmas with millions of particles.

Cette thèse porte sur la fonctionnalisation de surface par microstructuration laser. L’étude expérimentale a consisté à texturer des surfaces d’acier inoxydable avec une source laser impulsionnelle à fibre dopée Yb (1030 nm, 300 fs), dans le but de contrôler leur mouillabilité et de les rendre superhydrophobes. Par une optimisation des conditions d’irradiation, il est possible de conférer à la surface une structuration à double échelle de rugosité. Des structures d’une dizaine de micromètres sont réalisées par ablations successives selon un motif de lignes croisées, sur lesquelles se forment des nanostructures auto-organisées. La simulation du couplage de l’énergie dans la cible a permis de déterminer les paramètres opératoires pour limiter l’accumulation thermique en surface. L’étude fait clairement apparaître le rôle de la texturation dans l’apparition du caractère superhydrophobe de la surface, tout en soulignant l’influence des propriétés physico-chimiques du matériau. / This PhD thesis is about surface functionalization by laser microstructuring. The experimental study consists in texturing stainless steel surfaces with a pulsed Yb fibre laser source (1030 nm, 300 fs), in order to control their wettability and confer to them superhydrophobic properties. With an optimization of the irradiating conditions on the target, it is possible to confer to the surface a dual-scale roughness. By successive ablations according to a pattern of crossed lines, microstructures in the range of tens of micrometres are realized, on which self-organized nanostructures are superimposed. Simulation of the energy coupling in the material allows to determine the process parameters to be used, in order to limit the thermal accumulation and avoid the melting of the surface. This study reveals the role of the laser texturing in the apparition of the superhydrophobic character and emphasizes the influence of the physicochemical properties of the material.

Le laser à impulsions ultra-courtes constitue un procédé innovant et très avantageux pour la découpe de céramiques piézoélectriques PZT. Grâce à un fort confinement spatiotemporel de l’énergie au cours de l’interaction, ce système minimise les dégâts collatéraux et préserve l’intégrité physique du matériau sur des échelles micrométriques. Néanmoins, une propagation de faisceau mal maîtrisée, associée à des mécanismes d’interaction complexes fonction de la cible irradiée, peuvent impliquer de fortes disparités sur la qualité d’usinage. Dans le cadre d’une application industrielle donnée, ces travaux nous ont donc permis d’approfondir les principales étapes d’optimisation d’un tel procédé selon des critères de reproductibilité, de qualité et de rapidité. Pour cela, nous avons tout d’abord souligné l’influence des propriétés gaussiennes des faisceaux et de leur perturbation afin de définir la distribution énergétique au niveau des plans de focalisation. Aussi, la quantification de l’interaction via les critères de seuil et de taux d’ablation, d’incubation et de saturation a contribué à comprendre la réaction du matériau de manière macroscopique. Les problèmes méthodologiques inhérents à leurs calculs ont été mis en évidence et ont permis par la suite d’anticiper les formes d’usinage ainsi que les temps de procédé. Dans un second temps, l’optimisation des paramètres laser s’est appuyée sur des caractérisations aussi bien qualitatives pour l’aspect visuel que quantitatives avec l’estimation de la stoechiométrie et des contraintes résiduelles au niveau des flancs d’usinage. Nous avons en outre tiré profit de la piézoélectricité afin de développer une méthode d’observation in situ de la réponse à l’onde de choc laser contribuant à la compréhension des fissurations apparentes. Nous proposons au terme de ce travail un jeu de paramètres optimal pour la découpe de PZT assurant une bonne répétabilité du procédé tout en minimisant les défauts d’usinage comme la fissuration, les dépôts de surface et les irrégularités de bords. Des essais sur la mise en forme spatio-temporelle de faisceau sont enfin abordés principalement en tant que perspective d’accélération du procédé et encouragent son utilisation pour une future industrialisation / Lasers delivering ultrashort pulses are innovative and very attractive tools for cutting piezoelectric PZT ceramics. Thanks to an efficient spatiotemporal confinement of the energy during the interaction, these systems reduce collateral damage and preserve the physical integrity of the material on a micrometric scale. Nevertheless, uncontrolled beam propagation associated with complex interaction mechanisms depending on the irradiated target can involve large disparities on machining quality. In the context of an industrial application, this study describes the main steps of optimization of such a process according to criteria of reproducibility, quality and speed. To this purpose, we first pointed out the influence of Gaussian beam properties and their disturbance to define the energy distribution at focal planes. Thus, the quantification of the interaction with the ablation threshold, the ablation rate, incubation and saturation helped to understand the reaction of the material macroscopically. Methodological issues coming from their calculations have been highlighted while machining shapes and processing times were anticipated. Secondly, the optimization of laser parameters was based on both qualitative and quantitative characterizations. Electronic microscopy was rather used for visual appreciations whereas stoichiometry and residual stress estimations were employed to quantify the quality of side walls. We also took benefit from piezoelectricity to develop an in situ observation method which succeeded in detecting the electrical response to the laser shock wave and mainly contributed to the understanding of visible cracks. We finally propose an optimum set of parameters for cutting PZT ensuring good repeatability of the process while minimizing machining defects such as cracking, surface recast and jagged sides. Tests with spatiotemporal beam shaping were finally presented primarily as perspectives of processing time decrease so as to promote its use for future industrialization

Ein Ziel der Arbeit war die Entwicklung eines Verfahrens zur 3D-Positionierung auf Basis elektrooptischer Pseudostreckenmessung. Ein zweites Ziel war die Entwicklung eines Reflexgoniometers zur zweiachsigen Winkelmessung. Im Rahmen der Arbeit wurden die Grundlagen zur instrumentellen Umsetzung beider Verfahren erarbeitet, die Genauigkeitspotentiale ermittelt und mögliche Anwendungen für die einzelnen Schlüsseltechnologien und deren Kombination abgeleitet. In einer Prototyp-Entwicklung wurden Vorschläge für die wesentlichen Funktionselemente des räumlichen Weg- bzw. Winkelmesssystems gemacht. Hierzu gehören das kardanisch aufgehängte Etalon, die temperaturstabilisierte Laseroptik und die temperaturkalibrierte CCD der Winkelmesseinheit (Reflexgoniometer), die Systeme zur Erzeugung und Detektion ultrakurzer Laserpulse, eine elastische Optik, Möglichkeiten zur Formung des transversalen Strahlprofils, das TCSPC-System und die zur Auswertung und Kalibrierung notwendigen Algorithmen, wie z.B. die Autokollimation eines Lasers. ("Veröffentlicht von der Deutschen Geodätischen Kommission Reihe C (Dissertationen) unter der Nummer C 614 (München 2008; ISBN 3 7696 5053 0; 2; 144 S.") / One goal of the thesis was the development of a method for three-dimensional positioning based on electro-optical measurement of pseudo ranges. Another goal was the development of a reflex goniometer for biaxial angle measurement. Within the scope of this thesis the basics for the instrumental realisation of both methods were developed, the accuracy potentials were determined and possible applications for the separate key technologies and their combination were deduced. In a prototype development proposals were made for the main functional elements of the spatial distance and angle measurement systems. These include the gimbal mounted etalon, the temperature stabilised laser optics and the temperature calibrated CCD of the angle measurement device (reflex goniometer), the systems for creation and detection of ultrashort laser pulses, an elastic optical device, possibilities of transversal beam shaping, the TCSPC system and the algorithms which are necessary for analysis and calibration, e.g. the autocollimation of a laser.

A hybrid quantum-classical approach to the interaction of atomic clusters with intense laser fields in the vacuum ultra-violet (VUV) has been developed. Much emphasis is put on localized electrons, those quasi-free electrons which localize about the ions and screen them. These electrons set a time scale, which is used to interpolate between the quantum, rate based description of photon absorption by bound electrons and the classical, deterministic description of the cluster nano-plasma. Typical observables such as total energy absorption, electron and ion spectra are in very good agreement with the experimental findings. A scheme to probe the multi-electron motion in clusters with attosecond laser pulses is introduced. Conventional final state measurements in the energy domain cannot provide information about earlier states of the system due to the incoherent nature of the dynamics. Time-delayed attosecond pulses in the extreme ultra-violet (XUV) are used to probe the transient charging of the cluster ions during the interaction with the laser by measuring the kinetic energy of the electrons detached by the probe pulse. This information is otherwise lost at later times due to recombination. Knowledge about the transient charging would also shed more light on the still controversial subject of the energy absorption mechanisms in the VUV regime. Moving to shorter duration of the excitation, the characteristic time-scales for ionization and plasma equilibration are inversed. An attosecond laser pulse in the VUV regime creates a dense, warm nano-plasma far from equilibrium. Time-delayed attosecond pulses in the XUV probe then both the creation and the relaxation. The latter shows the breakup of the Bogoliubov hierarchy of characteristic times, indicating strongly-coupled plasma dynamics and drawing parallels to the relaxation of extended ultra-cold neutral plasmas with millions of particles.

Advanced polymeric materials, such as polyether ether ketones (PEEK), have been placed as direct substitutes for metals and ceramics in diverse applications, such as the machinery industry and biomedical engineering. Moreover, surface treatments allow the emergence of brand-new properties or the improvement of preexisting ones, such as friction, lubrication, wettability, cellular infiltration, or osseointegration. A paramount approach to achieving topographical modifications is by using laser micro/nanoprocessing techniques such as direct laser interference patterning (DLIP). Herein, PEEK foils are structured with DLIP method using ultrashort pulses. The influence of the pulse duration between 266 fs and 15 ps and the pulse-to-pulse overlap on the resulting surface topography and chemistry is assessed. As a result, well-defined line-like textures with a period of 5.8 μm and aspect ratios up to 0.88 are achieved. Furthermore, it is possible to explore and understand the behavior of surface phenomena such as swelling, increase/decrease of laser–material interaction onset, and laser-induced periodic surface structures formation. A comprehensive topographical and chemical characterization study demonstrates that these distinctive topographical features occur because of multiphoton absorption, incubation effects, and heat accumulation. These phenomena allow structuring polymeric substrates that are low-absorbing and challenging to pattern with conventional nanosecond infrared (IR) laser sources.