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Cette thèse porte sur la modélisation de l'ébullition qui joue un rôle important dans les vitessesde refroidissement des pièces, elle possède un volet numérique et un volet expérimental. Lessimulations et les expériences envisagées se situent à deux échelles. A l'échelle d'une ou quelquesbulles de vapeur, il s'agit de faire des simulations multiphasiques très précises en prenant encompte, la tension de surface, les calculs directs d'écoulement à grand nombre de Reynolds, etrendant compte du détachement et de la coalescences des bulles. Des observations expérimentalessont réalisées à la même échelle en contrôlant en surface la nucléation d'une bulle de vapeur àl'aide d'une caméra rapide. Des mesures de champs de vitesse par PIV et de température par twocolor LIF thermometry sont réalisées dans les mêmes conditions. Ceci a permit de confronter lacroissance, la dynamique et les formes des bulles observées et calculés. Les techniques numériquesles plus avancées sont utilisées : Eléments finis stabilisé VMS, level set, adaptation anisotropeet calcul intensif. Les modéles numériques proposés dans cette thèse permettent de passer àl'échelle macroscopique des pièces industrielles en considérant un film de vapeur (ou une phasede mélange liquide vapeur). L'enjeu supplémentaire étant de modéliser la turbulence induite parl'ébullition dans une approche de type CFD. / This thesis focuses on the modelling of boiling that plays an important role on the coolingand heat treatment in quenching processes, it has two components: numerical simulations andexperimental measurements. Both simulations and experiments are envisaged for two scales. Thefirst one concerns small scales: the scale of one or few bubbles. In this case, the focus is put onvery precise numerical simulations for multiphase flows taking into account the surface tension,the direct computations of flows at high Reynolds number, and on reflecting the detachmentand coalescence of bubbles. On that same scale, experimental observations are performed tocontrol, in the volume or at surface, the nucleation of a vapour bubble using a high speedcamera. Measurements of velocity fields by PIV and the temperature by PLIF are realizedunder the same conditions. This will allow us to compare the growth dynamics and shapesof bubbles observed and calculated. Advanced numerical methods are used to fulfil this task:VMS stabilized finite elements, level set, anisotropic adaptation and parallel computing. Thenumerical models proposed in this work are extended and also used to deal with macroscopicscales: at the level of industrial parts considering the vapour films (or a phase of liquid vapourmixture). The additional challenge resides in the modelling of turbulence induced by boiling ina CFD approach.

In chapter 3 of our paper we present equations of motion for continuous mass distribution subject to hydrodynamic forces in their most general form. We start with equations for discrete mass particles and then transform the equations so that it is appropriate for a continuous mass distribution. As we do that, new forms of interactions are generated and we successfully include these interactions, using the propagator theory, in the general form of our hydrodynamic equations for continuous mass distributions. We also took a deeper mathematical description of rotational flows. We were able to explain many physical phenomena successfully by our treatment of rotational flows in a more concrete and simple way, for example, the phenomenon of ripples that appear on ocean beaches and in desert sands. In chapter 4 we study the behavior of water surfaces. A liquid drop of water takes on a spherical shape because of the phenomenon of surface tension. A physical model based on the arrangement which the water molecules have on the surface is introduced to explain the above phenomenon. A mathematical model, as well as the physical model mentioned above, is introduced to describe the kind of forces involved on a wavy surface. The equations obtained describe the phenomenon of surface tension on a microscopic level very successfully. In chapter 5 we apply the results of chapters 3 and 4 to get an equation that gives a critical dynamical value which govern the interactions between the moving fluid and the dust particles residing on the ground. / Graduation date: 1996

La thèse porte sur l'étude de la convection capillaire (effet Marangoni) et son couplage avec la convection thermogravitationnelle. Le travail met en oeuvre des mesures de champ de vitesse par vélocimétrie laser, d'une part, et des simulations numériques de ces expériences, d'autre part. Des solutions asymptotiques sont également utilisées, et la transition de la convection stationnaire vers un état d'oscillations spatiales ou spatio-temporelles a été analysée. Le manuscript aborde également des situations impliquant l'effet de thermodiffusion, ainsi que les mouvements dans une bicouche de fluides immiscibles.

The scope of this thesis is micromanipulation in liquid media. This scientific field aims at understanding the relevant phenomena existing during the manipulation in a liquid of microcomponents having a size between $1,micrometer$ and a few millimeters. This work focuses on the study of surface tension forces in immersed media, because they have favorable scaling effect. The main idea is to use gas bubbles as actuation mean in a liquid, and requires to study the mechanical properties of these bubbles. The originality of the approach is the combination of two effects: surface tension and gas compressibility. The first step was the study of an efficient mean to generate a single bubble of predefined size. After a detailed review, it appeared that volume controlled bubble generation was a promising method. We have then developed a model to predict the size of a bubble, and emphasized the possible existence of a growing instability. An analytic dimensionless study allowed to define a criterion to predict the existence of this instability. The second step aimed at the mechanical characterization in quasi static equilibrium of a gas bubble caught between two solids. The purpose is to predict the force generated by the bubble, together with its stiffness. The model implemented allowed to infer interesting properties, notably a high compliance whose value is controllable by fluidic parameters. This compliance property being very important during micromanipulation, a demonstrator making use of gas bubbles has been designed and manufactured. It consists in a compliant microtable actuated by three bubbles. This work opens the way to new actuation or sensing means, using the transduction between fluidic and mechanic energy operated by a capillary bridge. / Cette thèse a pour contexte la micromanipulation en milieu liquide. Cette thématique scientifique vise à comprendre les phénomènes qui interviennent lors de la manipulation dans un liquide de microcomposants, dont la taille peut varier entre $1,micrometer$ et quelques millimètres. Les travaux de cette thèse se sont focalisés sur l'étude des forces de tension de surface en milieu immergé, car elles bénéficient d'effets d'échelle favorables. L'idée poursuivie est d'utiliser des bulles de gaz comme un moyen d'actionnement dans les milieux liquides, et nécessite d'étudier les propriétés mécaniques de ces bulles. L'originalité de l'approche repose sur la combinaison de deux effets : la tension de surface et la compressibilité du gaz. La première étape a été l'étude d'un moyen efficace pour générer une unique bulle de gaz de taille voulue. Après une analyse exhaustive, il est apparu que la génération de bulle par le contrôle en volume était une méthode prometteuse. Nous avons alors développé un modèle permettant de prédire la taille d'une bulle, et mis en évidence la possible existence d'une instabilité de la croissance de ces bulles. Une étude analytique adimensionnelle nous a permis de définir un critère pour prédire l'existence ou non de cette instabilité. La seconde étape a porté sur la caractérisation mécanique en régime quasi statique d'une bulle de gaz en contact avec deux solides. Le but étant de prédire la force générée par une bulle de gaz sur les solides ainsi que sa raideur. Le modèle implémenté a permis de déduire des propriétés intéressantes des bulles de gaz, notamment une grande compliance dont la valeur peut être contrôlée par des paramètres fluidiques. Cette propriété de compliance étant très recherchée en micromanipulation, un démonstrateur exploitant les bulles de gaz a été conçu. Il s'agit d'une microtable compliante actionnée par trois bulles. Ces travaux ouvrent la voie vers de nouveaux modes d'actionnement ou de capteur utilisant la transduction entre une énergie fluidique et mécanique opérée par un ménisque capillaire.

Adsorption-mediated self-assembly of nanoparticles at fluid interfaces, driven by reduction in interfacial energy, leads to stabilization of emulsions and foams and can be used for the bottom-up fabrication of functional nanostructured materials. Improved understanding of the parameters that control the self-assembly, the structure of nanoparticles at the interface, the barrier properties of the assembly and the rate of particle attachment and exchange is needed if such nanoparticle assemblies are to be employed for the design and fabrication of novel materials and devices. Here, I report on the use of dynamic surface tension (DST) measurements to probe the kinetics of irreversible adsorption and self-assembly of hydrophobic ethyl-cellulose (EC) nanoparticles at the air-water interface. Using thermodynamic arguments, I make a direct connection between the DST and the time-dependent surface coverage. I show that adsorption models appropriate for surfactants (e.g., Ward and Tordai model) break down for irreversible adsorption of nanoparticles, when the adsorption energy far exceeds the mean energy of thermal fluctuations (kBT) and surface blocking effects give rise to a steric barrier to adsorption. I show instead that irreversible adsorption kinetics are unequivocally characterized in terms of the adsorption rate constant and the maximum (jamming) coverage, both of which are determined on the basis of DST data using the generalized random sequential adsorption theory (RSA) for the first time. Novel accurate estimates of the adsorption energy of 42 nm and 89 nm EC nanoparticles are also provided. Coverage of the interface to the jamming limit of 91%, corresponding to a triangular lattice in 2D, is experimentally demonstrated. Colloidal solutions of EC nanoparticles are stabilized at neutral pH by electrostatic repulsive forces. Strong adsorption of these particles at an interface of like charge suggests the parallel action of attractive hydrophobic forces.

The Pressure-Volume-Temperature (PVT) for polymer/gas solutions is an important fundamental property of which accurate data measurement has not been reported until recently. The diffusivity, solubility, and surface tension are critical physical properties of polymer/gas solutions in understanding and controlling polymer processing such as, foaming, blending, and extracting reaction. However, the determination of these properties relies on accurate PVT data as a prerequisite. Due to the difficulties involved in measuring the specific volume while maintaining a sufficiently high pressure and temperature to achieve a single-phase polymer/gas solution, accurate PVT data or volume swelling measurement of polymer/gas solutions is not yet available. In this research, a new methodology was proposed and developed for direct measuring the PVT properties of polymer melts saturated with high-pressure gas at elevated temperatures. The ultimate goal is to develop and construct an apparatus that would provide more accurate fundamental properties through PVT measurement to the foaming industry, which is heavily involved with polymer/gas mixtures.

Studies of nucleation in freezing nanoparticles usually assume that the embryo of the solid phase is completely wet by the liquid and forms in the core of the droplet. However, recent experiments and computer simulations have suggested that some nanoparticles start nucleating at the liquid-vapor interface of the drop in a pseudoheterogeneous process. The goal of the present work is to propose phenomenological models suitable for the study of surface nucleation in nanoparticle systems that can be used to understand the contributions of the various surface phenomena, such as surface and line tensions, to the nucleation barrier.<p/> The nucleation barrier for the freezing of a 276 atom gold cluster is calculated using Monte Carlo simulation techniques while previous simulation studies of a 456 atom gold cluster are extended in order to find the probability that the embryo forms in the surface or core of the nanoparticle. These calculations confirm that the crystal embryo forms at the liquid-vapor interface. Geometric studies measuring the liquid-solid and solid-vapor surface areas of the embryo suggest that it changes shape as it becomes larger and grows in towards the core of the droplet.<p/> Three phenomenological models that are based on the capillarity approximation and can account for surface nucleation are proposed. These models highlight the importance of accounting for the surface curvature contributions related to the Tolman length and the presence of the three phase contact line in calculating the nucleation free energy barrier. In some cases, the models are able to reproduce the qualitative properties of the free energy barriers obtain from simulation but numerical fits of the models generally result in estimates of the solid-liquid surface tension that are lower than the values expected on the basis of partial wetting in the bulk.<p/> Finally, a semi-phenomenological model approach to nucleation is proposed where the usual phenomenological expression for the free energy barrier is retained, but where the geometric prefactors are obtained from molecular simulation of the embryo. This method is applied to nucleation in the gold cluster and to the freezing of a bulk Lennard-Jones liquid.<p/>

Studies of nucleation in freezing nanoparticles usually assume that the embryo of the solid phase is completely wet by the liquid and forms in the core of the droplet. However, recent experiments and computer simulations have suggested that some nanoparticles start nucleating at the liquid-vapor interface of the drop in a pseudoheterogeneous process. The goal of the present work is to propose phenomenological models suitable for the study of surface nucleation in nanoparticle systems that can be used to understand the contributions of the various surface phenomena, such as surface and line tensions, to the nucleation barrier.<p/> The nucleation barrier for the freezing of a 276 atom gold cluster is calculated using Monte Carlo simulation techniques while previous simulation studies of a 456 atom gold cluster are extended in order to find the probability that the embryo forms in the surface or core of the nanoparticle. These calculations confirm that the crystal embryo forms at the liquid-vapor interface. Geometric studies measuring the liquid-solid and solid-vapor surface areas of the embryo suggest that it changes shape as it becomes larger and grows in towards the core of the droplet.<p/> Three phenomenological models that are based on the capillarity approximation and can account for surface nucleation are proposed. These models highlight the importance of accounting for the surface curvature contributions related to the Tolman length and the presence of the three phase contact line in calculating the nucleation free energy barrier. In some cases, the models are able to reproduce the qualitative properties of the free energy barriers obtain from simulation but numerical fits of the models generally result in estimates of the solid-liquid surface tension that are lower than the values expected on the basis of partial wetting in the bulk.<p/> Finally, a semi-phenomenological model approach to nucleation is proposed where the usual phenomenological expression for the free energy barrier is retained, but where the geometric prefactors are obtained from molecular simulation of the embryo. This method is applied to nucleation in the gold cluster and to the freezing of a bulk Lennard-Jones liquid.<p/>

The Pressure-Volume-Temperature (PVT) for polymer/gas solutions is an important fundamental property of which accurate data measurement has not been reported until recently. The diffusivity, solubility, and surface tension are critical physical properties of polymer/gas solutions in understanding and controlling polymer processing such as, foaming, blending, and extracting reaction. However, the determination of these properties relies on accurate PVT data as a prerequisite. Due to the difficulties involved in measuring the specific volume while maintaining a sufficiently high pressure and temperature to achieve a single-phase polymer/gas solution, accurate PVT data or volume swelling measurement of polymer/gas solutions is not yet available. In this research, a new methodology was proposed and developed for direct measuring the PVT properties of polymer melts saturated with high-pressure gas at elevated temperatures. The ultimate goal is to develop and construct an apparatus that would provide more accurate fundamental properties through PVT measurement to the foaming industry, which is heavily involved with polymer/gas mixtures.