The propagation of intense picosecond laser pulses in air in the presence of strong nonlinear self-action effects and air ionization is investigated experimentally and numerically. The model used for numerical analysis is based on the nonlinear propagator for the optical field coupled to the rate equations for the production of various ionic species and plasma temperature. Our results show that the phenomenon of plasma-driven intensity clamping, which has been paramount in femtosecond laser filamentation, holds for picosecond pulses. Furthermore, the temporal pulse distortions in the picosecond regime are limited and the pulse fluence is also clamped. In focused propagation geometry, a unique feature of picosecond filamentation is the production of a broad, fully ionized air channel, continuous both longitudinally and transversely, which may be instrumental for many applications including laser-guided electrical breakdown of air, channeling microwave beams and air lasing.

Laser filamentation is a non-diffracting propagation regime consisting of an intense core that is surrounded by an energy reservoir. For laser ablation based spectroscopy techniques such as Laser Induced Breakdown Spectroscopy (LIBS), laser filamentation enables the remote delivery of high power density laser radiation at long distances. This work shows a quasiconstant filament-induced mass ablation along a 35 m propagation distance. The mass ablated is sufficient for the application of laser filamentation as a sampling tool for plasma based spectroscopy techniques. Within the scope of this study, single-shot ablation was compared with multi-shot ablation. The dependence of ablated mass on the number of pulses was observed to have a quasi-linear dependence on the number of pulses, advantageous for applications such as spectroscopy. Sample metrology showed that both physical and optical material properties have significant effects on the filament-induced ablation behavior. A relatively slow filament-induced plasma expansion was observed, as compared with a focused beam. This suggests that less energy was transferred to the plasma during filamentinduced ablation. The effects of the filament core and the energy reservoir on the filamentinduced ablation and plasma formation were investigated. Goniometric measurements of the filament-induced plasma, along with radiometric calculations, provided the number of emitted photons from a specific atomic transition and sample material. This work advances the understanding of the effects of single filaments on the ablation of solid materials and the understanding of filament-induced plasma dynamics. It has lays the foundation for further quantitative studies of multiple filamentation. The implications of this iv work extend beyond spectroscopy and include any application of filamentation that involves the interaction with a solid material

La propagation d’une impulsion laser femtoseconde dans un milieu condensé trans- parent tel que l’eau conduit, dans les conditions appropriées, à la manifestation de phénomènes d’optiques non linéaires regroupés sous le terme de filamentation laser. Le faisceau laser correspondant voit alors sa propagation métamorphosée sous la forme de filaments de lumière intense. Au coeur de ces filaments, l’irradiance considérable provoque l’ionisation des atomes du milieu et la génération de plasmas. Produit de manière spontanée et auto-régulée, ces plasmas ont la particularité de combiner une densité importante d’événements d’ionisation avec des effets thermo-mécaniques minimisés. Leurs propriétés intrinsèques font de ces plasma une source d’ionisation singulière tout particulièrement en ce qui concerne les sciences qui s’intéressent à l’étude des effets des radiations ionisantes. Entre autres, les sciences des radiations étudient la physique, la chimie et la biologie de l’action des rayonnements ionisants sur des systèmes d’intérêt biologique. Dans ce contexte, cette dissertation s’intéresse à la filamentation d’impulsions laser femtosecondes proches infrarouges en solution aqueuse. L’eau représentant la compo- sante majeure des systèmes d’intérêt biologique, une solution aqueuse constitue une approximation satisfaisante d’un échantillon biologique plus concret. Tout d’abord, l’étude de la physique de la filamentation laser a permis de mieux appréhender l’interaction des impulsions assujetties au processus de filamentation dans l’eau, primordiale pour l’identification des conditions d’irradiation propices à une meilleure maîtrise des conséquences de la génération des plasmas photo-induits. Les effets d’un rayonnement ionisant en solution aqueuse sont notamment véhiculés au travers de la chimie déclenchée par l’ionisation de l’eau, qui implique une interaction entre les espèces réactives produites et les solutés dilués en solutions. L’étude des conséquences de l’irradiation laser sur des solutés inorganiques a permis d’élucider la nature de cette chimie sous rayonnements. De surcroît, il a été démontré comment la malléabilité qu’offre l’utilisation d’un laser se répercute sur la capacité à moduler les conséquences de l’irradiation. Enfin, l’étude a été étendue à l’irradiation de molécules d’ADN diluées en solution aqueuse. L’analyse détaillée des dommages occasionnés à l’ADN a permis de mettre en exergue la présence de lésions complexes caractéristiques d’une irradiation par un faisceau intense de rayonnements ionisants. / Abstract : The present study is part in a new framework in radiobiology, introduced a decade ago: femtosecond laser-induced "cold" low density plasmas for the highly localized deposition of energy at sub-cellular scales in systems of biological interest. Since in aqueous solutions the action of such plasmas is equivalent to the deposition of a dose by ionizing radiation, plasma-mediated effects on solutes involve the radiation chemistry of water. This chemistry corresponds to the interaction of solutes with radical oxygen species as well as with secondary low energy electrons, produced by the plasma. Here, to better understand the radiation chemistry underlying the generation of low density plasmas in aqueous environments, we harnessed the multi-filamentation of powerful femtosecond laser pulses as a way to achieve a self-regulated production of spatially homogeneous low density plasma foci in water. The "cold" low density plasma micro-channels generated by the filamentation of the femtosecond laser pulses in aqueous solutions constitute a source of dense ionization. We studied the femtosecond laser filamentation in inorganic solutions to account for the radiation-assisted chemistry triggered by laser ionization in aqueous environment. We highlighted that the trivial optical control of the spatio-temporal distribution of light filaments in the irradiated sample resulted in the modulation of the corresponding radical chemistry. We concluded that these spatially and temporally resolved plasmas could be developed as a tool for the unprecedented control of chemistry under ionizing radiation. The addition of a spatial light modulator to control the filamentation process improves significantly our control on the spatio-temporal distribution of the laser-induced plasma channels. From a bundle of entangled random low density plasma channels, usually produced by the non-linear propagation of the powerful laser beam, we were able to obtain a programmable matrix of mono-filaments to achieve a more pervasive and homogeneous energy deposition. This method of irradiation allowed us to perform a detailed analysis to determine, quantify and compare the consequences of the laser irradiation with those of a conventional source of ionizing radiation (Gamma-Rays) on organic molecules (e.g. DNA) desolved in aqueous solutions. We showed that each filament behaves as an independent intense micro beam of ionizing radiation, that is capable of inducing complex DNA damage. We believe that a better understanding of the laser-induced plasma-mediated effects in aqueous solutions of biological interest will further the adoption of such laser-based ionisation sources, and that this unorthodox approach to radiation sciences will open new fields of investigation at the frontiers of radiation and laser-driven chemistry. Moreover, one of the principal conclusions of this thesis argues in favour of a shift of paradigm in radiation sciences, shuch that the consequences of ionising radiation would not only be considered for their injurious effects but also for the fine modulation of the functions of systems of biological interest. This sentiment paves the way for new emerging techniques and applications in biomedical fields.

<p>Laser-induced plasmas since their discovery in the 1960’s have found numerous applications in laboratories and industries. Their uses range from soft ionization source in mass spectroscopy, development of compact particle accelerator, and X-ray and deep UV radiation sources to diagnostic techniques such as laser-induced breakdown spectroscopy and laser electronic excitation tagging. In addition, the laser-induced plasma is important for studying of various nonlinear effects at beam propagation, such as laser pulse filamentation.</p> <p>This work deals with two challenging aspects associated with laser-induced plasmas. First is the study of Multi-Photon Ionization (MPI) as a fundamental first step in high-energy laser-matter interaction critical for understanding of the mechanism of plasma formation. The second is application of laser induced plasma for diagnostics of combustion systems.</p> <p>Numerous attempts to determine the basic physical constants of MPI process in direct experiments, namely photoionization rates and cross-sections of the MPI, were made; however, no reliable data was available until now, and the spread in the literature values often reached 2–3 orders of magnitude. This work presents the use of microwave scattering in quasi-Rayleigh regime off the electrons in the laser-induced plasma as method to measure the total number of electrons created due to the photoionization process and subsequently determine the cross-sections and rates of MPI. Experiments were done in air,<i> O₂, Xe, Ar, N₂, Kr</i>, and <i>CO</i> at room temperature and atmospheric pressure and femtosecond-laser pulse at 800 nm wavelength was utilized. Rayleigh microwave scattering (RMS) technique was used to obtain temporally resolved measurements of the electron numbers created by the laser. Numbers of electrons in the range 3 × 10⁸–3 × 10¹² were produced by the laser pulse energies 100–700 <i>μ</i>J and corresponding electron number densities down to about 10¹⁴ cm^-3 in the center of laser-induced spark were observed. After the laser pulse, plasma decayed on the time scale from 1 to 40 ns depending on the gas type and governed by two competing processes, namely, the creation of new electrons from ionization of the metastable atoms and loss of the electrons due to dissociative recombination and attachment to oxygen. </p> <p>Diagnostics of combustion at high pressures are challenging due to increased collisional quenching and associated loss of acquired signal. In this work, resonance enhanced multiphoton photon ionization (REMPI) in conjunction with measurement of generated electrons by RMS technique were used to develop diagnostics method for measuring concentration of a component in gaseous mixture at elected pressure. Specifically, the REMPI-RMS diagnostics was developed and tested in the measurements of number density of carbon monoxide (<i>CO</i>) in mixtures with nitrogen (<i>N₂</i>) at pressures up to 5 bars. Number of REMPI-induced electrons scaled linearly with <i>CO</i> number density up to about 5×10¹⁸ cm^-3 independently of buffer gas pressure up to 5 bar, and this linear scaling region can be readily used for diagnostics purposes. Higher <i>CO</i> number densities were associated laser beam energy loss while travelling through the gaseous mixture. Four (4) energy level model of <i>CO</i> molecule was developed and direct measurements of the laser pulse energy absorbed in the two-photon process during the passage through the <i>CO</i>/<i>N₂</i> mixture were conducted in order to analyze the observed trends of number of REMPI-generated electrons with <i>CO</i> number density and laser energy.</p>

<p>Constructive elastic microwave scattering, or, historically, coherent microwave scattering (CMS), refers to the inference of small plasma object characteristics via in-phase electromagnetic scattering – and has become a valuable technique in applications ranging from photoionization and electron-loss rate measurements to trace species detection, gaseous mixture and reaction characterization, molecular spectroscopy, and standoff measurement of local vector magnetic fields in gases through magnetically-induced depolarization. Notable advantages of the technique include a high sensitivity, good temporal resolution, low shot noise, non-intrusive probing, species-selectivity when coupled with resonance-enhanced multiphoton ionization (REMPI), single-shot acquisition, and the capability of time gating due to continuous scanning.</p> <p>Originally, the diagnostic was used for the measurement of electron total populations and number densities in collisional, weakly-ionized, and unmagnetized small plasma objects – so called collisional scattering. However, despite increased interest in recent years, the technique’s applicability to collisionless plasmas has remained relatively unexplored. This dissertation intends to expand upon the theoretical, mathematical, and experimental basis for CMS and demonstrate the constructive Thomson & Rayleigh scattering regimes for the first time. Furthermore, this work seeks to explore other novel and relevant capabilities of CMS including electron momentum-transfer collision frequency measurements via scattered phase information and spatially-resolved electron number characterizations of elongated plasma filament structures.</p> <p>This dissertation additionally leverages the technique to diagnose microplasmas and situations of particular interest. Primarily, photoionization (PI) – including UV resonance-enhanced multiphoton ionization, non-resonant visible PI, and mid-IR tunneling ionization in gaseous media. Such processes bear importance to studies on nonequilibrium plasmas, soft ionization in mass spectrometry, the development of compact particle accelerators, X-ray and deep UV radiation sources, laser-assisted combustion, laser-induced breakdown spectroscopy, species detection, mixture characterization and spectroscopy, studies on nonlinear beam propagation (filamentation, self-trapping and pulse splitting, dispersion, modulation instabilities), and so on. Finally, the application of CMS to ion thrusters is demonstrated.</p>