<p>Multiple industry applications, including combustion, flow control, and medicine, have leveraged nanosecond pulsed plasma (NPP) discharges to create plasma generated reactive species (PGRS). The PGRS are essential to induce plasma-assisted mechanisms, but the rate of generation and permanence of these species remains complex. Many of the mechanisms surrounding plasma discharge have been discovered through experiments, but a consistent challenge of time scales limits the plasma measurements. Thus, a well-constructed model with experimental research will help elucidate complex plasma physics. The motivation of this work is to construct a feasible physical model within the additional numerical times scale limitations and computational resources. This thesis summarizes the development of a one-moment fluid model for NPP discharges, which are applied due to their efficacy in generating ionized and excited species from vacuum to atmospheric pressure. </p><p>From a pulsed power perspective, the influence of pulse parameters, such as electric field intensity, pulse shape and repetition rate, are critical; however, the effects of these parameters on PGRS remain incompletely characterized. Here, we assess the influence of pulse conditions on the electric field and PGRS computationally by coupling a quasi-one-dimensional model for a parallel plate geometry, with a Boltzmann solver (BOLSIG+) used to improve plasma species characterization. We first consider a low-pressure gas discharge (3 Torr) using a five-species model for argon. <a>We then extend to a 23 species model with a reduced set of reactions for air chemistry remaining at low pressure.</a> The foundations of a single NPP is first discussed to build upon the analysis of repeating pulses. Because many applications use multiple electric pulses (EPs) the need to examine EP parameters is necessary to optimize ionization and PGRS formation. </p><p>The major goal of this study is to understand how the delivered EP parameters scale with the generated species in the plasma. Beginning with a similar scaling study done by Paschen we examine the effects of scaling pressure and gap length when the product remains constant for the two models. This then leads to our study on the relationship of pulsed power for different voltages and pulse widths of EPs. By fixing the energy delivered to the gap for a single pulse we determine that the electron and ion number densities both increased with decreasing pulse duration; however, the rate of this increase of number densities appeared to reach a limit for 3 ns. These results suggest the feasibly of achieving comparable outputs using less expensive pulse generators with higher pulse duration and lower peak voltage. Lastly, we study these outcomes when increasing the number of pulses and discuss the effects of pulse repetition and the electron temperature.</p><p>Future work will extend this parametric study to different geometries (i.e. pin-to-plate, and pin-to pin) and ultimately incorporate this model into a high-fidelity computational fluid dynamics (CFD) model that may be compared to spectroscopic results under quiescent and flowing conditions will be discussed.<br></p>

The use of supercontinuum light sources in different optical measurement methods, like microscopy or optical coherence tomography, has increased significantly compared to classical wideband light sources. The development of various optical measurement techniques benefits from the high brightness and bandwidth, as well as the spatial coherence of these sources. For some applications, only a portion of the broad spectral range can be used. Therefore, an increase of the spectral power density in limited spectral regions would provide a clear advantage over spectral filtering. This study describes a method to increase the spectral power density of supercontinuum sources by amplifying the excitation wavelength inside a nonlinear photonic crystal fiber (PCF). An ytterbium doped photonic crystal fiber was manufactured by a nanopowder process (drawn by the company fiberware) and used in a fiber amplifier setup as the nonlinear fiber medium. In order to characterize the fiber’s optimum operational characteristics, group-velocity dispersion (GVD) measurements were performed on the fiber during the amplification process. For this purpose, a notch-pass mirror was used to launch the radiation of a stabilized laser diode at 976 nm into the fiber sample for pumping. The performance of the fiber was compared with a conventional PCF. Finally, the system as a whole was characterized in reference to common solid state-laser-based photonic supercontinuum light sources. An improvement of the power density up to 7.2 times was observed between 1100 nm to 1380 nm wavelengths.

Supercontinuum light sources provide a high power spectral density with a high spatial coherence. Coherent octavespanning supercontinuum can be generated in photonic crystal fibers (PCFs) by launching short pulses into the fiber. In the field of optical metrology, these light sources are very interesting. For most applications, only a small part of the entire spectrum can be utilized. In biological tissue scattering, absorption and fluorescence limits the usable spectral range. Therefore, an increase of the spectral power density in limited spectral regions would provide a clear advantage over spectral filtering. This study describes a method to increase the spectral power density of supercontinuum sources by amplifying the excitation wavelength inside a nonlinear photonic crystal fiber (PCF). An all-fiber-based setup enables higher output power and power stability. An ytterbium-doped photonic crystal fiber was manufactured by a nanopowder process (drawn by the fiberware GmbH, Germany) and used in a fiber amplifier setup as the nonlinear fiber medium. In order to characterize the fiber’s optimum operational characteristics, group-velocity dispersion (GVD) measurements were performed. The performance of the fiber-based setup was compared with a free space setup. Finally, the system as a whole was characterized in reference to common solid state-laser-based supercontinuum light sources. An improvement of the power density was observed in the spectral range between 1100 nm to 1400 nm.

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Ce mémoire signe la fin de ma maîtrise dans le cadre du master Sciences et Technologies des Plasmas (STP), à l’Université Paul Sabatier de Toulouse, en partenariat avec l’Univer- sité de Montréal dans le cadre d’une double diplomation. L’objectif de cette double tutelle, portée par Ahmad Hamdan à Montréal et Flavien Valensi à Toulouse, est l’étude d’une décharge streamer en interaction avec une goutte d’eau au moyen du développement d’un modèle numérique. La goutte est positionnée entre deux électrodes pointes, le tout, sur un support en Téflon. Pour ce faire un modèle fluide permettant de suivre l’évolution spatio-temporelle des élec- trons, des ions positifs et des ions négatifs a été construit en python. L’équation dérive- diffusion est résolue, en 2D, pour chaque espèce, ainsi que l’équation de Poisson afin d’obtenir le champ électrique dans tout le domaine de calcul. Les coefficients de transport sont tabulés en fonction du champ électrique réduit dans l’hypothèse d’équilibre avec le champ électrique local. La photoionisation, jouant un rôle important pour la propagation du streamer positif à pression atmosphérique, a également était prise en compte au travers de la résolution de trois équations d’Helmholtz. Le modèle a été validé en comparant le terme source par impact électronique, supposé pro- portionnel à l’émission lumineuse, obtenu numériquement, à la lumière émise par la décharge enregistrée expérimentalement dans le domaine visible à l’aide d’une caméra ICCD. La dy- namique de la décharge a pu être étudiée grâce à l’évolution spatio-temporelle du champ électrique, de la densité électronique et de la densité de charge d’espace. L’influence de la constante diélectrique de la goutte sur la dynamique de la décharge a été ensuite étudiée. La répartition spatiale du champ électrique étant modifiée par le diélec- trique, son influence sur la décharge est importante. La vitesse de propagation des streamers est diminuée lorsque la permittivité de la goutte diminue ainsi que la valeur de la densité électronique dans le canal conducteur une fois formé. Enfin, l’angle de contact entre la goutte et le Téflon a été modifié. Les résultats ainsi obte- nus permettent de prédire le comportement de la décharge sur des géométries pouvant être rencontrées dans différentes situations expérimentales / This thesis marks the completion of my Master’s degree in the framework of the Plasma Sciences and Technologies (STP) program at the Paul Sabatier University of Toulouse, in partnership with the University of Montreal for a dual degree. The objective of this joint supervision, led by Ahmad Hamdan in Montreal and Flavien Valensi in Toulouse, is to study a streamer discharge interacting with a water droplet through the development of a numer- ical model. The droplet is positioned between two pointed electrodes, all placed on a Teflon substrate. To achieve this, a fluid model capable of tracking the spatiotemporal evolution of electrons, positive ions, and negative ions was constructed in Python. The drift-diffusion equation is solved in 2D for each species, along with the Poisson equation to obtain the electric field throughout the computational domain. Transport coefficients are tabulated as a function of the reduced electric field, assuming local equilibrium with the electric field. Photoionization, which plays a significant role in the propagation of positive streamers at atmospheric pres- sure, is also taken into account through the solution of three Helmholtz equations. The model was validated by comparing the source term due to electron impact, assumed to be proportional to the emitted light, obtained numerically, with the light emitted by the discharge recorded experimentally in the visible range using an ICCD camera. The discharge dynamics were studied through the spatiotemporal evolution of the electric field, electron density, and space charge density. The influence of the dielectric constant of the droplet on the discharge dynamics was then investigated. The spatial distribution of the electric field is modified by the dielectric, thus having a significant impact on the discharge. The streamer propagation velocity is reduced when the permittivity of the droplet decreases, as well as the value of the electron density within the formed conductive channel. Lastly, the contact angle between the droplet and Teflon was modified. The obtained re- sults allow predicting the behavior of the discharge on geometries encountered in different experimental situations.

The purpose of this dissertation is to — on occasion very literally — shine a light on processes that occur in non-thermal plasmas containing CO2, mostly for CO2 conversion. In particular, the focus lies on the transient behaviour of these discharges: how do these systems evolve over time before they settle in a (non-thermal) equilibrium. In addition to that, it analyses trends in the field of plasma-catalytic CO2 conversion as a whole to evaluate the current state-of-the-art, but also presents a new platform for the community to contribute and collaborate on, to facilitate cross-comparison between disparate experiments. The first part consists of experiments performed on: (a) an atmospheric pressure nanosecond repetitively pulsed (NRP) discharge for CO2 conversion, and (b) a test bed system for a remote CCP plasma source for plasma-enhanced atomic layer deposition (PE-ALD) of trimethylaluminium (TMA). The common theme in these experiments is a focus on the application of time-resolved, in situ diagnostics to study transient behaviour in the systems under investigation. The main diagnostics employed for such measurements are optical emission spectroscopy (OES) and laser induced fluorescence (LIF), which can provide complementary results when used in conjunction. In particular, this work presents the following results: A study of the evolution of emission from an NRP discharge (using OES), establishing both electron densities (by Stark broadening of atomic oxygen and carbon lines) and gas temperatures (by the N2 second positive system) as the discharge evolves from a breakdown phase to a spark phase. It furthermore explores the changes to these properties when operating in burst mode, where a subsequent pulse experiences a memory effect from the preceding one, which has been shown to be conducive to efficient conversion in literature. A study into the effect on energy efficiency of CO2 conversion by alternating the power modulation in an NRP discharge. Crucially, using CET-LIF (collisional energy transfer LIF) and OES it is shown that while power deposition to the discharge occurs in the order of 100 ns in the discharge, CO2 dissociation occurs on a timescale beyond a microsecond. This indicates that instead of direct electron impact, molecular-excitation kinetics play an important role under these conditions for CO2 dissociation. By shortening the time between pulses in a burst (down to 33 us in the work), these mechanisms can be further enhanced, by prolonging the quasi-‘metastable’ state of the system. The application of LIF in a PE-ALD process plasma along with OES, where diffusion profiles were measured close to the substrate surface with local time-resolved measurements of the OH ground state density. These indicate that the investigated surface reactions finish on a timescale of 100 ms, faster than would be indicated by OES which effectively measures emission from the bulk plasma after diffusion of reaction products away from the surface. The second part of this work is an open access database on plasma(-catalytic) CO2 conversion that is instrumental in identifying and verifying trends in experimental data, but also stresses the importance of rigorous reporting of essential parameters in literature. The approach in literature is diverse: some studies focus more on a mechanistic understanding of the fundamental processes, whilst others already focus on process tailoring and optimization for industrial applications. Trends observed in earlier review papers are observed as well and can now be trivially reproduced. The database platform (https://db.co2pioneer.eu) is put forward as a new tool for the community to easily cross-compare and contextualize experimental outcomes and strongly encourages new contributions. Based on the 196 papers included at the time of publication, a number of observations and recommendations can already be made. Chief among those is a clear and present need in the field for a more fundamental understanding of plasma-catalysis interaction, to develop techniques and criteria that are properly suited to test the synergy of both, rather than relying on methods from e.g. traditional thermal-catalysis. Also in this instance, local, time-resolved diagnostics may play a key role, but their implementation will be challenging.

Ce travail de thèse a eu pour but de développer des nouvelles sources lasers, oscillateurs et ampli?cateurs, construites autour des ?bres dopées aux ions ytterbium. Ces systèmes lasers génèrent des fortes puissances moyennes. L’oscillateur réalisé délivre des impulsions courtes (<10 ns) avec des énergies de l’ordre du milliJoule. Le système fonctionne à des cadences variables (10-100 kHz) avec un faisceau polarisé, monomode dont la largeur spectrale est inférieure à 0.1 nm. A?n d’avoir de plus fortes puissances crêtes et des impulsions courtes, deux types d’ampli?- cateurs ont été étudiés. Les résultats expérimentaux que nous avons obtenus sont en accord avec le modèle numérique développé. Le premier système ampli?e un microlaser émettant à 1064 nm dans une ?bre dopée ytterbium. Des puissances crêtes supérieures à 500 kW ont été obtenues avec des impulsions de l’ordre de la nanoseconde et une cadence comprise entre 1 kHz et 30 kHz. Le second ampli?cateur est construit autour d’un oscillateur à ?bre dopée ytterbium déclenché injecté dans une deuxième ?bre qui constitue l’ampli?cateur. L’originalité de ce système réside dans le cou- plage de deux cavités. Nous avons alors en sortie deux faisceaux cohérents, polarisés, monomode, indépendamment ajustables en énergie. En?n, nous avons utilisé les sources lasers développées, qui présentent des caractéristiques spec- trales, modales, énergétiques adéquats pour effectuer la conversion de fréquence. Des ef?cacités de l’ordre de 64 % et 38 % ont été atteintes respectivement en doublage et en triplage. Les faisceaux en sortie de ces systèmes possèdent des remarquables caractéristiques spatiales et temporelles. / This work presents the development of oscillators and ampli?ers build around new ytterbium rod type ?ber. These ?ber systems generate high average power generation. The oscillator makes it possible to deliver well linearly polarized, almost TEM 00 mode, and millijoule-level nanosecond pulses at a tunable repetition rate (10-100 kHz). The spectral bandwidth was shown to be less than 0.1 nm. To achieve higher peak power and shorter pulses, two types of ampli?ers have been developed and characterized. The experimental results we obtain, do well agree with the numerical simulations we developped. The ?rst system ampli?es in a rod type ?ber the nanosecond pulses yielded by a microlaser working at 1064 nm wavelength injected . Its provides pulses with a high peak power system (500 kW). Its repetition rate was tuned from 1 kHz to 30 kHz. The second ampli?er was built using a Q-switched ytterbium doped ?ber oscillator injected in a second ?ber which acts as ampli?er. In this original system the two cavities are coupled. It delivers two nanosecond pulses that are coherent, polarized, almost TEM00 single mode beams and that can have independently tunable pulse energies. We have shown that these oscillators and ampli?ers can be easily doubled and tripled in fre- quency. Very high ef?ciency of about 64 % and 38 % have been achieved respectively at 2? and 3?. These outputs have been to have remarquable spatial and temporal characteristics.