Dans ce travail de thèse, des méthodes de simulation numérique ont été utilisées afin de modéliser, à l’échelle moléculaire,l’interaction entre des aérosols carbonés et diverses molécules de l’atmosphère.L’objectif était de caractériser les propriétés physico-chimiques de ces aérosols, qui jouent un rôle majeur dans le climat, en particulier via leur capacité à former des noyaux de condensation pour les molécules d’eau. En premier lieu, les techniques de la dynamique moléculaire ont été appliquées à la détermination de l’organisation d’agrégats d’acide carboxylique sur lesquels sont adsorbées des molécules d’eau. Les résultats montrent une influence à la fois de la température, du taux d’humidité et du type d’acide considéré sur le comportement global des agrégats. Par contre, il a été montré qu’un mélange binaire d’acides n’a que peu d’influence sur ce comportement. En second lieu, des techniques de simulation moléculaires quantiques, à la fois statiques et dynamiques, ont été appliquées à l’étude de la chloration de surfaces de suie, modélisées par de grands HAP, ainsi qu’à la caractérisation de leur affinité pour les molécules d’eau. Les résultats ont montré une forte propension de Cl, Cl2 et HCl à former des HAP chlorés à la faveur de la présence de défauts structurels. Ces structures chlorées présentent une forte hydrophilicité, ce qui pourrait expliquer la nature fortement hygroscopique de suies émises lors d’incendies industriels. / In this PhD work, molecular simulation methods have been used in order to model, at the molecular scale, the interaction between carbonaceous aerosols andvarious atmospheric species. The aim wasto characterize the physico-chemical properties of these aerosols, which play a major role in climate forcing, in particular through their ability to act as cloud condensation nuclei.First, molecular dynamics techniques have been applied to determine the structure of carboxylic acid aggregates on which water molecules are adsorbed. The results of our simulations show an influence of the temperature, of the humidity and of the type of carboxylic acid considered on the global behavior of the aggregates. By contrast,a mixture of different types of acid molecules has no influence on this behavior. Secondly, quantum molecular simulation techniques have been applied to study the chlorination of soot surfaces, modeled by large PAHs, and their behavior with respect to water molecules adsorption. The results show a strong propensity of Cl, Cl2and HCl species to form chlorinated PAHsthanks to the presence of structural defects.These chlorinated structures show as trong hydrophilicity, which may explain the strong hygroscopic nature of soots emitted by industrial fires.

O presente trabalho simula numericamente os efeitos na transferência de calor radiativa a partir da injeção de fuligem no interior de uma câmara cilíndrica que opera com chama turbulenta. São resolvidas equações de conservação de massa, de energia, de quantidade de movimento, da variância da flutuação de temperatura, de espécies químicas gasosas e de fuligem para um problema físico conhecido, partindo da combustão da mistura de metano e ar dentro de uma câmara com dimensões e condições de contorno já exploradas em outros trabalhos a fim de possibilitar comparações de resultados. Para a turbulência é utilizado o modelo k - E padrão. Na modelagem das interações turbulência-radiação, é considerada a correlação combinada entre coeficiente de absorção e temperatura e a autocorrelação de temperatura. Foram adotados os modelos de Eddy Break-Up – Arrhenius para a combustão, utilizando a reação de combustão em duas etapas. O método de ordenadas discretas, considerando a soma-ponderada-de-gases-cinza (WSGG – do inglês: weighted-sum-of-graygases) é utilizado para calcular o termo fonte de calor radiativo. A dependência espectral das propriedades radiativas do meio participante foi modelada pelo método WSGG, que permite a solução de problemas com concentração variável das espécies participantes com alto nível de confiabilidade. A simulação da injeção de fuligem foi realizada alterando as condições de contorno do problema, resolvendo-se os cálculos de forma acoplada. Os resultados obtidos após a injeção externa da fuligem foram comparados com simulações que apenas consideravam a formação natural e a posterior oxidação das partículas. Foram analisados os campos do termo fonte de calor radiante em toda a câmara, que mostraram aumento sensível da radiação após a injeção ser considerada. Comparou-se também o fluxo de calor que atinge as paredes da câmara, como principal análise do presente trabalho, indicando que mesmo injetando pequenas quantidades de fuligem, há um aumento no fluxo de calor. O campo de temperatura não apresentou alterações consideráveis, apenas reduzindo-se a temperatura máxima no interior da câmara. De uma forma geral, o efeito da fuligem é mais significativo nas regiões de alta temperatura. / This work simulates numerically the effects on radiative heat transfer after the soot injection into a cylindrical combustion chamber that operates with turbulent flames. A known physical problem of burning methane with air inside a chamber is considered. The dimensions and boundary conditions were already considered in other papers to enable comparisons between the results. Conservation equations for mass, momentum, gaseous chemical species and soot, energy, and temperature variance equations, are solved. The turbulence is modeled by standard k -E model. Consideration of TRI (Turbulence-Radiation Interactions) effects is made through a methodology that considers both cross-correlation between absorption coefficient and temperature self correlation. The combustion model is Eddy Break-Up – Arrhenius, with two steps for the combustion reaction. The radiative heat source term is calculated with the discrete ordinates method, considering the weighted-sum-of-gray-gases model (WSGG). The spectral dependence of the participant media radiative properties was modeled by WSGG method, which allows the solution of problems with varying concentration of the participating species with high level of reliability. The simulation of soot injection was performed by changing the contour conditions of the problem. The calculation was solved in a coupled way. The results obtained after foreign soot injection were compared with simulations which only considered the natural formation and subsequent oxidation of the particles. The fields of the radiative heat source term showed significant increase of radiation after the soot injection was considered. The radiative heat flow that reaches the chamber walls is compared between the cases, as one of the main analysis of this work. It indicates that even when small amounts of soot injection are considered, there is an increase in the radiative heat flow to the walls. The temperature behavior showed no significant change, except on reducing the maximum temperature within the chamber. In general, the effects on the radiative heat transfer after the soot injection are greater in the high temperature areas.

O presente trabalho simula numericamente os efeitos na transferência de calor radiativa a partir da injeção de fuligem no interior de uma câmara cilíndrica que opera com chama turbulenta. São resolvidas equações de conservação de massa, de energia, de quantidade de movimento, da variância da flutuação de temperatura, de espécies químicas gasosas e de fuligem para um problema físico conhecido, partindo da combustão da mistura de metano e ar dentro de uma câmara com dimensões e condições de contorno já exploradas em outros trabalhos a fim de possibilitar comparações de resultados. Para a turbulência é utilizado o modelo k - E padrão. Na modelagem das interações turbulência-radiação, é considerada a correlação combinada entre coeficiente de absorção e temperatura e a autocorrelação de temperatura. Foram adotados os modelos de Eddy Break-Up – Arrhenius para a combustão, utilizando a reação de combustão em duas etapas. O método de ordenadas discretas, considerando a soma-ponderada-de-gases-cinza (WSGG – do inglês: weighted-sum-of-graygases) é utilizado para calcular o termo fonte de calor radiativo. A dependência espectral das propriedades radiativas do meio participante foi modelada pelo método WSGG, que permite a solução de problemas com concentração variável das espécies participantes com alto nível de confiabilidade. A simulação da injeção de fuligem foi realizada alterando as condições de contorno do problema, resolvendo-se os cálculos de forma acoplada. Os resultados obtidos após a injeção externa da fuligem foram comparados com simulações que apenas consideravam a formação natural e a posterior oxidação das partículas. Foram analisados os campos do termo fonte de calor radiante em toda a câmara, que mostraram aumento sensível da radiação após a injeção ser considerada. Comparou-se também o fluxo de calor que atinge as paredes da câmara, como principal análise do presente trabalho, indicando que mesmo injetando pequenas quantidades de fuligem, há um aumento no fluxo de calor. O campo de temperatura não apresentou alterações consideráveis, apenas reduzindo-se a temperatura máxima no interior da câmara. De uma forma geral, o efeito da fuligem é mais significativo nas regiões de alta temperatura. / This work simulates numerically the effects on radiative heat transfer after the soot injection into a cylindrical combustion chamber that operates with turbulent flames. A known physical problem of burning methane with air inside a chamber is considered. The dimensions and boundary conditions were already considered in other papers to enable comparisons between the results. Conservation equations for mass, momentum, gaseous chemical species and soot, energy, and temperature variance equations, are solved. The turbulence is modeled by standard k -E model. Consideration of TRI (Turbulence-Radiation Interactions) effects is made through a methodology that considers both cross-correlation between absorption coefficient and temperature self correlation. The combustion model is Eddy Break-Up – Arrhenius, with two steps for the combustion reaction. The radiative heat source term is calculated with the discrete ordinates method, considering the weighted-sum-of-gray-gases model (WSGG). The spectral dependence of the participant media radiative properties was modeled by WSGG method, which allows the solution of problems with varying concentration of the participating species with high level of reliability. The simulation of soot injection was performed by changing the contour conditions of the problem. The calculation was solved in a coupled way. The results obtained after foreign soot injection were compared with simulations which only considered the natural formation and subsequent oxidation of the particles. The fields of the radiative heat source term showed significant increase of radiation after the soot injection was considered. The radiative heat flow that reaches the chamber walls is compared between the cases, as one of the main analysis of this work. It indicates that even when small amounts of soot injection are considered, there is an increase in the radiative heat flow to the walls. The temperature behavior showed no significant change, except on reducing the maximum temperature within the chamber. In general, the effects on the radiative heat transfer after the soot injection are greater in the high temperature areas.

O presente trabalho simula numericamente os efeitos na transferência de calor radiativa a partir da injeção de fuligem no interior de uma câmara cilíndrica que opera com chama turbulenta. São resolvidas equações de conservação de massa, de energia, de quantidade de movimento, da variância da flutuação de temperatura, de espécies químicas gasosas e de fuligem para um problema físico conhecido, partindo da combustão da mistura de metano e ar dentro de uma câmara com dimensões e condições de contorno já exploradas em outros trabalhos a fim de possibilitar comparações de resultados. Para a turbulência é utilizado o modelo k - E padrão. Na modelagem das interações turbulência-radiação, é considerada a correlação combinada entre coeficiente de absorção e temperatura e a autocorrelação de temperatura. Foram adotados os modelos de Eddy Break-Up – Arrhenius para a combustão, utilizando a reação de combustão em duas etapas. O método de ordenadas discretas, considerando a soma-ponderada-de-gases-cinza (WSGG – do inglês: weighted-sum-of-graygases) é utilizado para calcular o termo fonte de calor radiativo. A dependência espectral das propriedades radiativas do meio participante foi modelada pelo método WSGG, que permite a solução de problemas com concentração variável das espécies participantes com alto nível de confiabilidade. A simulação da injeção de fuligem foi realizada alterando as condições de contorno do problema, resolvendo-se os cálculos de forma acoplada. Os resultados obtidos após a injeção externa da fuligem foram comparados com simulações que apenas consideravam a formação natural e a posterior oxidação das partículas. Foram analisados os campos do termo fonte de calor radiante em toda a câmara, que mostraram aumento sensível da radiação após a injeção ser considerada. Comparou-se também o fluxo de calor que atinge as paredes da câmara, como principal análise do presente trabalho, indicando que mesmo injetando pequenas quantidades de fuligem, há um aumento no fluxo de calor. O campo de temperatura não apresentou alterações consideráveis, apenas reduzindo-se a temperatura máxima no interior da câmara. De uma forma geral, o efeito da fuligem é mais significativo nas regiões de alta temperatura. / This work simulates numerically the effects on radiative heat transfer after the soot injection into a cylindrical combustion chamber that operates with turbulent flames. A known physical problem of burning methane with air inside a chamber is considered. The dimensions and boundary conditions were already considered in other papers to enable comparisons between the results. Conservation equations for mass, momentum, gaseous chemical species and soot, energy, and temperature variance equations, are solved. The turbulence is modeled by standard k -E model. Consideration of TRI (Turbulence-Radiation Interactions) effects is made through a methodology that considers both cross-correlation between absorption coefficient and temperature self correlation. The combustion model is Eddy Break-Up – Arrhenius, with two steps for the combustion reaction. The radiative heat source term is calculated with the discrete ordinates method, considering the weighted-sum-of-gray-gases model (WSGG). The spectral dependence of the participant media radiative properties was modeled by WSGG method, which allows the solution of problems with varying concentration of the participating species with high level of reliability. The simulation of soot injection was performed by changing the contour conditions of the problem. The calculation was solved in a coupled way. The results obtained after foreign soot injection were compared with simulations which only considered the natural formation and subsequent oxidation of the particles. The fields of the radiative heat source term showed significant increase of radiation after the soot injection was considered. The radiative heat flow that reaches the chamber walls is compared between the cases, as one of the main analysis of this work. It indicates that even when small amounts of soot injection are considered, there is an increase in the radiative heat flow to the walls. The temperature behavior showed no significant change, except on reducing the maximum temperature within the chamber. In general, the effects on the radiative heat transfer after the soot injection are greater in the high temperature areas.

Le rayonnement joue un rôle fondamental dans les problèmes d'incendie puisque c'est le mode dominant de transfert de chaleur entre la flamme et le milieu environnant. Il contrôle la pyrolyse, et donc la puissance de flamme, et la vitesse de croissance de l'incendie. Étudier les flammes de diffusion contrôlées par les forces de flottabilité est une première étape pour comprendre et de prédire les incendies. Le principal objectif de ce travail est de modéliser le transfert radiatif et les processus de production/destruction de la suie dans ce type de flammes. Premièrement, différents modèles de propriétés radiatives des gaz ont été comparés dans des configurations tests. Il est apparu que le modèle FSCK couplé avec le schéma de mélange de Modest et Riazzi est le meilleur compromis entre précision et temps de calcul, ce modèle étant un bon candidat pour être implémenté dans des codes CFD traitant des problèmes d'incendie. Dans un second temps, un modèle de formation/oxydation des suies semi-détaillé, considérant l'acétylène et le benzène comme précurseurs, a été validé dans des flammes de diffusion laminaires de type coflow sur une large gamme d'hydrocarbures (C1-C3) et pour différentes conditions. Ensuite, le FSCK et le modèle de formation/destruction ont été appliqués pour simuler des feux de nappe de méthane et de propane aux échelles du laboratoire et intermédiaire. Les structures de flamme prédites ainsi que les flux radiatif transférés au milieu environnant ont montré un bon accord avec les résultats expérimentaux disponibles. Finalement, les interactions entre le rayonnement et la turbulence ont été quantifiées. / The radiative heat transfer plays an important role in fire problems since it is the dominant mode of heat transfer between flames and surroundings. It controls the pyrolysis, and therefore the heat release rate, and the growth rate of the fire. In the present work a numerical study of buoyant diffusion flames is carried out, with the main objective of modelling the thermal radiative transfer and the soot formation/destruction processes. In a first step, different radiative property models were tested in benchmark configurations. It was found that the FSCK coupled with the Modest and Riazzi mixing scheme was the best compromise in terms of accuracy and computational requirements, and was a good candidate to be implemented in CFD codes dealing with fire problems. In a second step, a semi-empirical soot model, considering acetylene and benzene as precursor species for soot nucleation, was validated in laminar coflow diffusion flames over a wide range of hydrocarbons (C1-C3) and conditions. In addition, the optically-thin approximation was found to produce large discrepancies in the upper part of these small laminar flames. Reliable predictions of soot volume fractions require the use of an advanced radiation model. Then the FSCK and the semi-empirical soot model were applied to simulate laboratory-scale and intermediate-scale pool fires of methane and propane. Predicted flame structures as well as the radiant heat flux transferred to the surroundings were found to be in good agreement with the available experimental data. Finally, the interaction between radiation and turbulence was quantified.

Cette thèse consiste en l'étude expérimentale et numérique des processus de formation des particules de suie au sein des flammes laminaires non-pré-mélangées et partiellement prémélangées sous l'influence d'un champ magnétique ou d'une stimulation acoustique. Dans une premiére étape, la capacité du code CIAO à prédire la fraction volumique de suie dans une flamme axisymétrique est étudiée. Par la suite, deux flammes subissant une stimulation acoustique ont été étudiées. Les résultats peuvent être utilisés pour améliorer les modèles de suie futurs, en particulier concernant les différentes échelles temporelles de la chimie en phase gazeuse, et la formation d'hydrocarbures polyaromatiques (PAH) et de suie couplée avec des flux transitoires. Pour étudier la formation des particules de suie sous l'influence de gradients de champ magnétique, un brûleur de type Santoro est utilisé. Les techniques de mesure utilisées dans le cadre de cette thèse sont l'imagerie directe à haute cadence, la technique Background Oriented Schlieren (BOS) et la méthode d'Absorption/Emission Modulée (MAE). Une augmentation de la fraction volumique de suie intégrée a été mise en évidence lorsque le gradient de champ magnétique est ascendant. Une analyse de stabilité linéaire locale appliquée à l'écoulement non-visqueux est présentée pour une flamme sous l'influence de la perturbation magnétique envisagée. Le gradient de champ magnétique provoque alors une réduction du taux d'amplification. De fait, l'étude est complété par l'identification d'un domaine où les flammes qui oscillent naturellement peuvent être stabilisées et contrôlées par des gradients de champ magnétique. / In this thesis light is shed on the soot formation processes in laminar coflow flames influenced by magnetic field gradients and acoustic forcing. Both influences have been assessed experimentally and numerically. First, the CIAO in-house code's ability to predict soot volume fraction fields in a steady coflow flame is studied. Then, two acoustically forced cases were studied. These findings are used to improve future soot models, especially, concerning the different time scales of gas phase chemistry and the formation of polycyclic aromatic hydrocarbons (PAH) and soot coupled with unsteady flows. To investigate soot formation under magnetic field gradients, a Santoro type burner is used. The measurement techniques applied in the course of this thesis are high-speed luminosity measurements, Background Oriented Schlieren (BOS) and one- and two-color Modulated Absorption/Emission (MAE) techniques. The magnetic field impact on soot formation was first studied experimentally in steady laminar flames. A scaling of soot production similar to the increased integrated soot volume fraction with increased oxygen content in the coflow was documented. A local inviscid stability analysis is presented for an ethylene coflow flame to investigate the flame's response to small perturbations of the mean velocity, temperature, fuel, and oxygen massfraction under magnetic field exposure. The magnetic field is found to reduce the perturbations' growth rate. The magnetic field study is completed by identifying a domain where naturally oscillating flames can be stabilized and controlled by magnetic field gradients.

Les travaux s'inscrivent dans le développement de catalyseurs conducteurs ioniques à base de zircone stabilisée à l'oxyde d'yttrium (YSZ) pour l'oxydation des suies dans les filtres à particules (FAP) qui équipent les véhicules Diesel. L'oxydation de la suie sur YSZ a été observée à l'échelle nanométrique par microscopie électronique en transmission environnementale. La réaction d'oxydation se déroule à l'interface (20-40 nm) entre le catalyseur et la suie, l'activité étant liée au nombre de points de contact. Nous avons associé un vecteur d'oxygène mobile, l'argent, à YSZ. Les résultats montrent une synergie entre YSZ et les nanoparticules d'argent qui promeut l'activité notamment en cas de contact grossier avec la suie. Des expériences isotopiques d'échanges et d'oxydation ont démontré que l'argent active l'intégration de l'oxygène gazeux dans le réseau de YSZ. La caractérisation des propriétés physicochimiques des nanoparticules d'argent dispersées sur différents oxydes (une autre zircone yttriée aux propriétés différentes : YSZb, ZrO2, CeZrO2, SiO2) a permis de relier les performances catalytiques avec la teneur d'argent métallique en surface. Des tests de vieillissement hydrothermal ont montré que la formulation supportée sur YSZb présente une activité maintenue en contact médiocre avec la suie et une faible perte en argent. Des mini-FAPs imprégnés de catalyseur ont ensuite été testés sur un banc de gaz synthétiques capable de produire des particules de suie en suspension. L'activité des formulations catalytiques une fois mises en forme ainsi que leur capacité de filtration ont été évaluées. Un mini-FAP contenant la formulation Ag/YSZb oxyde les suies dès 350°C et s'auto-régénère (oxydation des suies plus rapide que leur collecte) dès 450°C / This study deals with the development of ionic conductive catalysts based on yttria-stabilized zirconia for soot oxidation in Diesel Particle Filter (DPF). Soot oxidation was observed at the nanoscale using Environmental Transmission Electron Microscopy. Reaction was shown to occur at the interface between YSZ and soot, ranging from 20 to 40 nm, and activity was related to the number of contact points between soot and catalyst. In order to promote activity, we associated to YSZ an oxygen carrier: silver, under the form of silver nanoparticles (AgNPs) scattered over YSZ surface. Results display a synergy between YSZ and AgNPs, allowing for the promotion of soot oxidation under poor contact conditions. Isotopic exchange and oxidation experiments demonstrated AgNPs promote oxygen integration into YSZ lattice. Characterizations of supported AgNPs over different oxides such as YSZb (displaying different properties than YSZ), ZrO2, SiO2, CeZrO2, indicate that the soot oxidation activity is related to the amount of metallic silver species on the oxide surface. Hydrothermal ageing tests indicate that Ag/YSZb formulation displays a stable activity in poor contact conditions and a low silver loss. Baby-DPF (1 inch diameter, 3 inches length) were impregnated with silver-supported catalysts and tested on a synthetic gas bench producing a gas stream containing suspended soot particles. Soot oxidation activity and filtration efficiency were measured. A baby-FAP containing the Ag/YSZb formulation was shown to oxide soot at a temperature as low as 350°C and to induce self-regeneration (soot oxidation overcoming the collection) at 450°C

L’objectif de cette étude était de développer une nouvelle génération de catalyseurs, dits électrochimiques, capables d’abaisser la température de régénération des filtres à particules, et de diminuer les coûts du post-traitement des moteurs Diesel, en évitant notamment une surconsommation en carburant. Pour cela, un banc de mesure a été développé où de forts moyens analytiques pour les phases gazeuses (GC et analyseur de NOx), particulaires (spectromètre de masse à aérosols AMS) et de caractérisations physiques des aérosols (SMPS, Scanning Mobility Particle Sizer) ont été couplés. Le catalyseur électrochimique développé est composé d’un catalyseur oxyde de type pérovskite La0.5Sr0.23Ag0.27MnO3±δ (noté LSAM), en contact avec un électrolyte solide conducteur par les ions O2-, la zircone dopée à l’oxyde d’yttrium (YSZ). L’enduction de ce catalyseur électrochimique directement dans les canaux d’un filtre à particule (FAP) en céramique (SiC) a montré des performances permettant d’abaisser la température de régénération des FAP de 100°C voire de 260°C selon le flux de régénération. Ces performances sont le résultat d’un effet de synergie entre les phases de la pérovskite LSAM et du conducteur ionique YSZ / The aim of this study was to develop a new generation of catalysts, called electrochemical, which can lower the regeneration temperature of the particulate filter, and reduce post-treatment costs of Diesel engines, especially avoiding over-consumption of fuel. For this, a test bench has been developed where strong analytical analyzer for gas phases (GC and Nox analyzer), for particles (aerosol mass spectrometer AMS) and for physical characterization of aerosols (SMPS, Scanning Mobility Particle Sizer) have been coupled. The electrochemical catalyst developed is composed of a perovskite catalyst La0.5Sr0.23Ag0.27MnO3±δ (denoted LSAM), in contact with a solid electrolyte conductor by O2-ions, yttria stabilised zirconia (YSZ). The coating of the electrochemical catalyst directly into the channels of a particulate filter (DPF) showed performance to lower the DPF regeneration temperature of 100°C or even 260°C depending of the regeneration flow. These performances are the result of a synergistic effect between the phases of the perovskite LSAM and YSZ ionic conductor

This work deals with carbon materials and using them in electrochemical energy sources. Object of this work was to prepare carbon materials and investigate their electrical properties. The theoretical part objects of the carbon materials, their properties, application in electrochemical energy sources and measurement methods used in experimental part. Experimental part describes the preparation of the electrodes with various carbon materials and summarizes the results of measurements.

Chaque année, une quantité de 107tonnes de suie est produite à l'échelle mondiale. Le carbone-suie dans l'atmosphère a des effets graves sur le changement climatique et la santé humaine. Les impacts dépendent de nombreux facteurs comme les composés organiques adsorbés, le vieillissement et les processus de mélange. Par conséquent, afin de réduire la quantité de suie émise, outre l'examen des facteurs mentionnés, les études de la cinétique de formation, de la structure et des propriétés optiques des suies sont également essentielles. Il existe plusieurs méthodes optiques dans les études sur la suie. La spectroscopie Raman occupe un rôle particulier puisqu'elle est un outil puissant pour l'étude structurale des matériaux carbonés grâce à sa sensibilité aux structures à l’échelle moléculaire. Dans ce travail, des sections Raman différentielles de suies et quelques autres particules carbonées ont été mesurées pour progresser vers la spectroscopie Raman quantitative de ces particules. Les suies produites par des flammes d'éthylène pré-mélangées à basse pression ont été étudiées par mesure Raman ex-situ sur des films déposés et des mesures Raman in-situ (enligne) dans la phase gazeuse. La combinaison de la spectroscopie Raman de suies échantillonnées sur substrat avec les spectroscopies infrarouge et optique et la microscopie électronique en transmission a permis de progresser sur l'interprétation des spectres Raman de suie. Les mesures en phase gazeuse, obtenues pour la première fois, fournissent de nouvelles informations sur la naissance des suies et leurs structures dans les flammes à basse pression avec, par exemple, la détection d'une grande quantité d'atomes de carbones hybridés sp lors de la formation et de la croissance des premières suies. Ces étude s’ouvrent la voie à la détection et à l'analyse des suies directement en phase gazeuse et à leur détection quantitative dans l’atmosphère au travers de leurs spectres Raman. / Every year, an amount of 107 tons of soot is produced on the world scale. Soot, as part of atmospheric black carbon, has serious impacts on climate change and human health. The impacts depend on many factors including adsorbed compounds, aging and mixing processes. Therefore in order to reduce the soot amount, besides considering these mentioned factors, the study of formation kinetics, structure and optical properties is also essential. There are several methods applied in soot investigations. Raman spectroscopy plays a particular role as it is a powerful tool for structural investigation of the carbon-based materials because it is sensitive to molecular structures. In this work, differential Raman cross sections of soot and some other carbonaceous particles were measured to progress toward quantitative Raman spectroscopy. Soot particles produced by premixed ethylene flames at a low pressure were investigated by ex-situ Raman measurement on deposited films and in-situ(online) Raman measurement in the gas phase. Combination of the Raman spectroscopy of soot sampled on substrates with infrared and optical spectroscopy and transmission electron microscopy allowed progressing on the interpretation of soot Raman spectra. The online gas phase measurements provided a novel view on soot birth and structures in low pressure flames with, for instance, the detection of a large amount of sp hybrized carbon atoms during nascent soot growth. These studies pave the way to soot detection and analysis directly and quantitatively in the atmosphere.