This dissertation addresses the analysis of partially premixed flame configurations and the detection and characterization of their local flame regimes. First, the identification of flame regimes in experimental data is intensively discussed. Current methods for combustion regime characterization, such as the flame index, rely on 3D gradient information that is not accessible with available experimental techniques. Here, a method is proposed for reaction zone detection and characterization, which can be applied to instantaneous 1D Raman/Rayleigh line measurements of major species and temperature as well as to the results of laminar and turbulent flame simulations, without the need for 3D gradient information. Several derived flame markers, namely the mixture fraction, the heat release rate and the chemical explosive mode, are combined to detect and characterize premixed versus non-premixed reaction zones. The methodology is developed and evaluated using fully resolved simulation data from laminar flames. The fully resolved 1D simulation data are spatially filtered to account for the difference in spatial resolution between the experiment and the simulation, and experimental uncertainty is superimposed onto the filtered numerical results to produce Raman/Rayleigh equivalent data. Then, starting from just the temperature and major species, a constrained homogeneous batch reactor calculation gives an approximation of the full thermochemical state at each sample location. Finally, the chemical explosive mode and the heat release rate are calculated from this approximated state and compared to those calculated directly from the simulation data. After successful validation, the approach is applied to Raman/Rayleigh line measurements from laminar counterflow flames, a mildly turbulent lifted flame and turbulent benchmark cases. The results confirm that the reaction zones can be reliably detected and characterized using experimental data. In contrast to other approaches, the presented methodology circumvents uncertainties arising from the use of limited gradient information and offers an alternative to known reaction zone identification methods. Second, this work focuses on the flame structure of partially premixed dimethyl ether (DME) flames. DME flames form significant intermediate hydrocarbons in the reaction zone and are classified as the next more complex fuel candidate in research after methane. To simulate DME combustion processes, accurate predictions by computational combustion models are required. To evaluate such models and to identify appropriate flame regimes, numerical simulations are necessary. Therefore, fully resolved simulations of laminar dimethyl ether flames, defined by different levels of premixing, are performed. Further, the qualitative two-dimensional structures of the partially premixed DME flames are discussed and analyses are carried out at selected slices and compared to each other as well as to experimental data. Further, the flamelet/progress variable (FPV) approach is investigated to predict the partially premixed flame structures of the DME flames. In the context of the FPV approach, a rigorous analysis of the underlying manifold is carried out based on the newly developed regime identification approach and an a priori analysis. The most promising flamelet look-up table is chosen for the fully coupled tabulated chemistry simulations and the results are further compared to the fully resolved simulation data.

<div>Laser-absorption spectroscopy (LAS) is widely used for providing non-intrusive and quantitative measurements of gas properties (such as temperature and absorbing species mole fraction) in combustion environments. However, challenges may arise from the line-of-sight nature of LAS diagnostics, which can limit their spatial resolution. Further, time-resolution of such techniques as scanned direct-absorption or wavelength-modulation spectroscopy is limited by the scanning speed of the laser and the optical bandwidth is often limited by a combination of a laser's intrinsic tunability and its scanning speed. The work presented in this dissertation investigated how recent advancements in mid-IR camera technology and lasers can be leveraged to expand the spatial, temporal, and spectral measurement capabilities of LAS diagnostics. Novel laser-absorption imaging and ultrafast laser-absorption spectroscopy diagnostics are presented in this dissertation. In addition, the high-pressure combustion chamber (HPCC) and high-pressure shock tube (HPST) were designed and built to enable the study of, among others, energetic material combustion, spectroscopy, non-equilibrium and chemistry using optical diagnostics.<br></div><div><br></div>

Cette thèse est consacrée à l’amélioration des capacités de prédiction des émissions d’oxydes d’azote (NO et NO2) des foyers de combustion aéronautiques. Les travaux, exclusivement numériques, consistent d’abord dans une étude de la cinétique chimique responsable des émissions polluantes. Cetteétude conduit à l’écriture d’un modèle, nommé NOMANI (pour Nitrogen Oxide emission model with one-dimensional MANIfold), basé sur l’approche PCM-FPI (pour Presumed Conditional Moments - Flame Prolongation of ILDM) avec une variable de progrès additionnelle afin calculer l’avancement de la chimie azotée une fois la chimie carbonée à l’équilibre. Différentes validations sur des configurations laminaires simples puis des flammes de laboratoire de Sandia sont présentées. Les résultats en terme de structure de flamme et d'émission de monoxyde d’azote sont confrontés aux mesures expérimentales. Le dernier volet de ces travaux, disponible uniquement dans la version confidentielle du manuscrit, consiste dans le développement d’un modèle de prédiction de polluants associé au modèle TF-LES (pour Thickening Flame for Large Eddy Simulation). Le modèle développé est ensuite appliqué à des calculs d’une chambre de combustion aéronautique. / This thesis is focused on the prediction capabilities of nitrogen oxides (NO and NO2) for numerical tools applied to aeronautical combustion chambers. The modeling work is based on a study of the chemical kinetic that produced the pollutant emissions. This study leads to a model, called NOMANI (Nitrogen Oxide emission model with one-dimensional MANIfold), based on PCM-FPI (Presumed Conditional Moments - Flame Prolongation of ILDM) with an additional progress variable to compute the NO evolution once the carbon chemistry is at the equilibrium. Several benchmarks and test-cases (laminar and turbulent flames) are gathered in this study : Sandia flame have been computed and satisfactory comparisons with measurements are obtained. The last part of this work, only available in the confidential version of the manuscript, is the development of a model to predict pollutant associated with the model TF-LES (for Thickening Flame for Large Eddy Simulation). This model is then applied to computations of a aeronautical combustion chambers.

La dynamique des flammes de prémélange est étudiée par deux approches numériques différentes. La première résout les équations compressibles de Navier-Stokes avec une chimie simplifiée (DNS). Afin de réduire les coûts de calcul, nous analysons et développons un schéma numérique à grille décalée. Le traitement des ondes acoustiques aux sorties est connu pour rendre les flammes cylindriques légèrement carrées. Ces déformations non-physiques sont expliquées en mettant en évidence la modélisation insuffisamment précise de l'accélération du fluide lorsque l'écoulement est oblique à la sortie. Une étude paramétrique et statistique de flammes turbulentes est menée en 2D et une simulation parallèle 3D est réalisée dans un domaine de (3cm)3. En considérant la flamme infiniment mince, l'approche EEM diminue considérablement les coûts de calcul. Les mêmes simulations sont réalisées et comparées aux résultats de DNS pour tester la capacité du modèle EEM à fournir des résultats quantitatifs. / We study premixed flame dynamics using DNS and EEM approaches. DNS solves compressible Navier-Stokes equations with simplified chemistry. To reduce computational costs and increase efifciency, we analyse and develop a modified staggered scheme. Treatment of acoustic waves at boundaries is known to slightly square cylindrical flames. We try to explain these unphysical distortions by highlighting the poor modeling of fluid acceleration when mainstrean is transverse to outow. A parametric and statistical study of expanding flames is carried out in 2D and also for an expanding (3cm)3 flame. The EEM approach models the flame as an infinitely thin interface. This perturbative strategy dramatically decreases cpu costs. Simulations are carried out and compared to DNS results to check the ability of EEM modeling to give quantitative results.

La combustion stratifiée, qui consiste à brûler un mélange carburant/oxydant inhomogène, et la combustion diluée, consistant à ajouter une quantité limitée de gaz brûlés, sont deux technologies utilisées dans les moteurs à piston pour réduire leur consommation. Cette thèse est dédiée à l’étude de l’allumage dans ces deux types de milieux en régimes laminaire et turbulent. Un nouveau schéma cinétique pour la combustion propane/air a été dérivé et combiné à deux approches de modélisation différentes : la chimie complexe et une approche de chimie tabulée de type FPI. Dans le cas laminaire, les deux approches de modélisation donnent des résultats similaires et un modèle simple a mis en évidence l’importance de la dynamique des gaz frais et des gaz brûlés sur le développement du noyau. Dans le cas turbulent, plusieurs techniques d’analyse ont montré la dépendance de la vitesse absolue de la flamme au champ de vitesse moyen et la décorrélation des fluctuations locales de richesse. / Stratified combustion, which consists in burning an inhomogeneous fuel/air mixture, and diluted combustion, which consists in adding a limited quantity of burnt gases, are two technologies used in internal combustion engines to reduce fuel consumption. This Ph.D is devoted to the study of ignition in these two types of combustion in laminar and turbulent regimes. A new kinetic scheme for propane/air combustion has been derived and combined to two modeling approaches: finite-rate chemistry and an FPI tabulated chemistry approach. In the laminar case, both approaches give similar results and a simplified model has highlighted the importance of fresh and burnt gases dynamics on the kernel development. In the turbulent case, several techniques of analysis have shown the dependency of absolute flame speed on the mean fluid velocity and the lack of correlation to the local equivalence ratio.

Malgré l'augmentation constante des ressources informatiques dédiées au calcul scientifique, simuler des écoulements réactifs mettant en jeu une chimie complexe reste aujourd'hui encore un véritable challenge. L'objectif de cette thèse est le développement de la méthode Hybrid Transported-Tabulated Chemistry (HTTC), destinée aux simulations DNS/LES de flammes avec des mécanismes cinétiques détaillés, en offrant un temps de calcul acceptable. Cette nouvelle approche consiste à transporter les espèces majoritaires de l'écoulement, tandis que les espèces minoritaires sont extraites d'une table chimique. La méthode HTTC a été implémentée dans un code DNS/LES et validée sur des flammes 1D de méthane et de kérosène, mettant en évidence une réduction extrêmement importante du temps de calcul, comparé aux solveurs classiques de chimie détaillée. HTTC a ensuite été mis en œuvre avec succès sur des flammes triples de méthane en présence de forts gradients de fraction de mélange. L'impact des méthodes choisies pour prolonger la table chimique et pour calculer les variables de contrôle, utilisées pour paramétrer la table, a été étudiée avec une attention particulière. Un très bon accord a été trouvé avec les résultats de référence, obtenus avec un solveur de chimie détaillée. / Even if significant progress is being made to improve the power of high-performance computers, the numerical simulation of reactive flows involving complex chemistry is still a challenging task. The objective of this work is the development of the Hybrid Transported-Tabulated Chemistry method (HTTC), designed for the DNS/LES simulations of flames with detailed kinetic mechanisms, with an acceptable cost. This novel approach combines the transport of the main species in the flow with the tabulation of the radical species. It has been implemented in a DNS/LES code and validated on 1D methane and kerosene flames. The cost of the simulations has been considerably decreased, compared to classic detailed chemistry solvers. Then, simulations of methane edge flames, featuring large gradients of mixture fraction, have been performed with HTTC. In particular, the impact of the methods used to extend the chemical tables and to compute the control variables have been analyzed in details. A very good agreement has been found by comparison with detailed chemistry.

This dissertation addresses the analysis of partially premixed flame configurations and the detection and characterization of their local flame regimes. First, the identification of flame regimes in experimental data is intensively discussed. Current methods for combustion regime characterization, such as the flame index, rely on 3D gradient information that is not accessible with available experimental techniques. Here, a method is proposed for reaction zone detection and characterization, which can be applied to instantaneous 1D Raman/Rayleigh line measurements of major species and temperature as well as to the results of laminar and turbulent flame simulations, without the need for 3D gradient information. Several derived flame markers, namely the mixture fraction, the heat release rate and the chemical explosive mode, are combined to detect and characterize premixed versus non-premixed reaction zones. The methodology is developed and evaluated using fully resolved simulation data from laminar flames. The fully resolved 1D simulation data are spatially filtered to account for the difference in spatial resolution between the experiment and the simulation, and experimental uncertainty is superimposed onto the filtered numerical results to produce Raman/Rayleigh equivalent data. Then, starting from just the temperature and major species, a constrained homogeneous batch reactor calculation gives an approximation of the full thermochemical state at each sample location. Finally, the chemical explosive mode and the heat release rate are calculated from this approximated state and compared to those calculated directly from the simulation data. After successful validation, the approach is applied to Raman/Rayleigh line measurements from laminar counterflow flames, a mildly turbulent lifted flame and turbulent benchmark cases. The results confirm that the reaction zones can be reliably detected and characterized using experimental data. In contrast to other approaches, the presented methodology circumvents uncertainties arising from the use of limited gradient information and offers an alternative to known reaction zone identification methods. Second, this work focuses on the flame structure of partially premixed dimethyl ether (DME) flames. DME flames form significant intermediate hydrocarbons in the reaction zone and are classified as the next more complex fuel candidate in research after methane. To simulate DME combustion processes, accurate predictions by computational combustion models are required. To evaluate such models and to identify appropriate flame regimes, numerical simulations are necessary. Therefore, fully resolved simulations of laminar dimethyl ether flames, defined by different levels of premixing, are performed. Further, the qualitative two-dimensional structures of the partially premixed DME flames are discussed and analyses are carried out at selected slices and compared to each other as well as to experimental data. Further, the flamelet/progress variable (FPV) approach is investigated to predict the partially premixed flame structures of the DME flames. In the context of the FPV approach, a rigorous analysis of the underlying manifold is carried out based on the newly developed regime identification approach and an a priori analysis. The most promising flamelet look-up table is chosen for the fully coupled tabulated chemistry simulations and the results are further compared to the fully resolved simulation data.

[pt] Dinâmica dos Fluidos Computacional (CFD) é frequentemente aplicada ao estudo da combustão, permitindo otimizar o processo e controlar a emissão de poluentes. Entretanto, reproduzir o comportamento observado nos sistemas de engenharia tem uma elevada carga computacional. Para superar este custo, técnicas de aprendizagem de máquinas, tais como modelos de ordem reduzida (ROM), têm sido aplicadas a várias aplicações de engenharia com o objetivo de criar modelos para sistemas complexos com custo computacional reduzido. Aqui, o ROM é criado usando dados de simulação de chama laminar não pré-misturada de CFD, decompondo-os, e depois aplicando um algoritmo de aprendizagem de máquinas, criando um ROM estático. Este trabalho analisa o efeito de cinco abordagens diferentes de pré-processamento de dados sobre o ROM, sendo estas: (1) as propriedades tratadas como um sistema desacoplado ou como um sistema acoplado, (2) sem normalização, (3) com temperatura e velocidade normalizadas, (4) todas as propriedades normalizadas, e (5) o logaritmo da espécie química. Para todos os ROM construídos são analisados a energia do processo de redução e a reconstrução dos campos das propriedades da chama. Em relação a análise da energia da redução, o ROM acoplado, exceto o ROM (4), e o ROM do logaritmo convergem rapidamente, semelhante ao ROM da temperatura desacoplado, enquanto o ROM da espécie química minoritária desacoplado exibe uma lenta convergência, tal como o ROM acoplado com todas as propriedades normalizadas. Assim, a aprendizagem é atingida com um número menor de modos para a ROM (2), (3) e (5). Quanto à reconstrução dos campos de propriedades, nota-se que existem regiões de fração mássica negativa, o que sugere que a metodologia do ROM não preserva a monotonicidade ou a delimitação das propriedades. A abordagem do logaritmo mostra que estes problemas são superados e reproduzem os dados originais. / [en] Computational fluid dynamics (CFD) is often applied to the study of combustion, enabling to optimize the process and control the emission of pollutants. However, reproducing the behavior observed in engineering systems has a high computational burden. To overcome this cost, machine learning techniques, such as reduced order models (ROM), have been applied to several engineering applications aiming to create models for complex systems with reduced computational cost. Here, the ROM is created using CFD laminar non premixed flame simulation data, decomposing it, and then applying a machine learning algorithm, creating a static ROM. This work analyzes the effect of five different data pre-processing approaches on the ROM, these being: (1) the properties treated as an uncoupled system or as a coupled system, (2) without normalization, (3) with temperature and velocity normalized, (4) all properties normalized, and (5) the logarithm of the chemical species. For all ROM constructed are analyzed the energy of the reduction process and the reconstruction of the flame properties fields. Regarding the reduction energy analysis, the coupled ROM, except the ROM (4), and the logarithm ROM converges faster, similarly to the uncoupled temperature ROM, whereas the uncoupled minor chemical species ROM exhibits a slower convergence, as does the coupled ROM with all properties normalized. So, the learning is achieved with a smaller number of modes for the ROM (2), (3) and (5). As for the reconstruction of the property fields, it is noted that there are regions of negative mass fraction, which suggest that the ROM methodology does not preserve the monocity or the boundedness of the properties. The logarithm approach shows that these problems are overcome and reproduce the original data.

Τα τελευταία χρόνια, η φασματοσκοπία πλάσματος επαγόμενο από λέιζερ (LIBS) έχει προσελκύσει μεγάλο ερευνητικό ενδιαφέρον καθώς αποτελεί μία πειραματικά απλή και αποτελεσματική τεχνική, η οποία παρέχει τη δυνατότητα λήψης μετρήσεων για απευθείας ποιοτική και ποσοτική στοιχειακή ανάλυση. Η τεχνική LIBS στηρίζεται στη δημιουργία σπινθήρα/πλάσματος μέσω ισχυρά εστιασμένης δέσμης λέιζερ στην επιφάνεια ή στο εσωτερικό του δείγματος, στην ακόλουθη διέγερση και ατομοποίηση των στοιχείων του στόχου και στην τελική καταγραφή και φασματοσκοπική ανάλυση της εκπεμπόμενης ακτινοβολίας του πλάσματος. Λόγω των πολλών πλεονεκτημάτων που συγκεντρώνει η τεχνική, το LIBS έχει προταθεί για πληθώρα πρακτικών, τεχνικών και τεχνολογικών εφαρμογών σε ένα ευρύ φάσμα ερευνητικών πεδίων. Από την άλλη μεριά, στον τομέα της καύσης, η ποσότητα καυσίμου σε ένα εύφλεκτο μίγμα είναι αντικείμενο μείζονος σημασίας καθώς επηρεάζει σημαντικά την απόδοση των χημικών διεργασιών και την παραγωγή και εκπομπή ρύπων. Επομένως, δημιουργείται η ανάγκη ανάπτυξης μίας γρήγορης και μη παρεμβατικής διαγνωστικής τεχνικής για τη μέτρηση της περιεκτικότητας του καυσίμου τοπικά στη φλόγα με καλή τόσο χωρική όσο και χρονική ανάλυση. Στα πλαίσια της παρούσας διδακτορικής διατριβής, η τεχνική LIBS η οποία συγκεντρώνει όλα αυτά τα πλεονεκτήματα χρησιμοποιήθηκε για αυτό το σκοπό. Κατά τη διάρκεια των πειραμάτων, χρησιμοποιήθηκαν πηγές λέιζερ διάρκειας παλμών ns και fs, ενώ τα συστήματα καύσης που μελετήθηκαν ήταν φλόγες υδρογονανθράκων-αέρα, στρωτής και τυρβώδους ροής, απλής και συνθετότερης γεωμετρίας. Από τα LIBS φάσματα φλογών διαφορετικής σύστασης, προέκυψε λοιπόν ότι υπάρχει μία ισχυρή εξάρτηση μεταξύ των εντάσεων διαφόρων φασματικών γραμμών με το λόγο ισοδυναμίας. Επομένως, μέσω της συσχέτισης αυτής μπορεί να επιτευχθεί με μεγάλη ακρίβεια τόσο η μέτρηση της περιεκτικότητα σε καύσιμο φλογών άγνωστης σύστασης όπως επίσης και η μέτρηση της κατανομής του καυσίμου τοπικά μέσα σε όλη την έκταση της φλόγας παρέχοντας σημαντικές πληροφορίες για την δομή της. Τέλος, εφαρμόστηκε μία παραπλήσια διαγνωστική τεχνική, κατά την οποία η διηλεκτρική κατάρρευση του μέσου ήταν αποτέλεσμα ενός ηλεκτρικού σπινθήρα: electrical Spark Induced Breakdown Spectroscopy (SIBS) όπου και πραγματοποιήθηκε η συγκριτική μελέτη της ακτινοβολίας του πλάσματος επαγόμενο μέσω οπτικής και ηλεκτρικής διέγερσης. / Laser induced breakdown spectroscopy (LIBS) has attracted a lot of scientific interest during the last two decades as it is generally considered to be an experimentally simple and efficient laser-based technique which can perform real-time, qualitative and quantitative elemental analysis. The basic idea of LIBS is the creation of spark/plasma through tight focusing of a laser beam on the surface or into a sample, the subsequent excitation and atomization of the species of the sample at the location where the spark is formed and the final detection and spectroscopic analysis of the emitted radiation from the decaying plasma. Seeing the numerous advantages holding the technique, LIBS has been proposed for many practical, technical and technological applications in various scientific areas. On the other hand, in the field of combustion, the proportion of fuel in a combustible mixture is of great importance as it strongly affects the efficiency of the chemical processes and the production of soot emissions. Therefore, there is a continuously increasing need for the development of a rapid and non-perturbative diagnostic technique for the determination of the fuel content locally in the flame structure with good spatial and temporal resolution. Ιn the present dissertation, LIBS technique which offers such advantages has been applied for combustion diagnostics purposes. During the experiments, laser systems with pulse duration in the scale of ns and fs have been applied as excitation sources, while the combustible mixtures under investigation were hydrocarbon-air flames, of laminar and turbulent flow with simple and more complicated structures. From the LIBS spectra in flames of different compositions, it was exhibited that there is a strong dependence of the intensities of various spectral lines on the equivalence ratio, which demonstrates that the precise determination of the amount of fuel can be performed. Also based on this correlation, the determination of the equivalence ratio locally everywhere within the flame can be achieved giving useful information about its structure. Finally, a similar diagnostic technique has been employed. The dielectric breakdown is held using a spark generator and the technique is called electrical Spark Induced Breakdown Spectroscopy (SIBS). The emitted light of the two plasmas induced by optical and electrical excitation was collected and a comparative study was performed.

Le risque d’explosion des mélanges H2/air revêt toujours une importance cruciale pour la gestion des accidents graves dans les centrales nucléaires. Des critères expérimentaux ont été proposés dans les années 2000 par Dorofeev et al. afin de déterminer les conditions nécessaires à l’accélération de flamme et à la TDD. Ce travail de thèse a l’objectif de mieux comprendre les mécanismes d’accélération des flammes de prémélange H2/air et de fournir une solide base de données expérimentales pour la validation des codes utilisés pour les études de sûreté. Les expériences ont été menées dans un tube muni d’obstacles (taux de blocage entre 0.3 et 0.6) avec un diamètre interne de 12 cm et une longueur d’environ 5 m. Les effets de la pression initiale et de la dilution en azote sur des mélanges pauvres en H2 ont été étudiés. Les résultats montrent que la pression favorise l’accélération seulement pour les mélanges les plus réactifs et que la surpression induite par la combustion est directement proportionnelle à la pression initiale. Les interactions flamme-choc ainsi que les instabilités thermo-diffusives jouent un rôle important sur la propagation de flamme. Une nouvelle technique a été développée dans le but d’obtenir une représentation plus fine du profil de vitesse de flamme. Des mesures d’absorption IR résolues dans le temps ont été effectuées en dopant le mélange avec un alcane. Le profil de vitesse a été obtenu en mesurant la variation d’extension du gaz frais pendant l’avancement de la flamme. Enfin, des analyses préliminaires ont été menées pour la conception d’un nouveau dispositif expérimental pour l’étude des effets de la combustion sur des structures en acier inox. / Flame acceleration and explosion of hydrogen/air mixtures remain key issues for severe accident management in nuclear power plants. Empirical criteria were developed in the early 2000s by Dorofeev and colleagues providing effective tools to discern possible FA or DDT scenarios. The objectives of the present work are to better understand the mechanisms of acceleration for premixed H2/air flames and to provide a solid base of experimental data for the validation of the codes used for safety analyses. The experiments were performed in an obstacles-laden tube (blockage ratio between 0.3 and 0.6) with 120 mm internal diameter and about 5 m length. The effects of the initial pressure and the nitrogen dilution on lean H2 mixtures have been studied. The results show that pressure promote flame acceleration only for highly reactive mixtures. Moreover, the overpressure induced by the combustion is directly proportional to the initial pressure. Besides, flame-shock interactions and thermo-diffusive instabilities play an important role in flame acceleration. A new technique to track the flame position along the tube has been developed in order to obtain a finer representation of the flame velocity profile. The method consists in performing time-resolved IR absorption measurements by doping the mixture with an alkane. The velocity profile is then derivedby measuring the variation of the extension in depth of the unburnt gas along the tube axis. Finally, analyses on the effects of combustion generated loads on stainless steel structures were performed in order to provide preliminary results for the design of a new experimental device.