Airborne infectious diseases remain a major global health threat. The primary vector for their transmission is coarse and fine droplets, known as bioaerosols, exhaled from infected individuals during natural respiratory maneuvers, such as breathing, coughing and sneezing. Unfortunately, our current knowledge of the mechanisms by which these exhaled bioaerosols are formed in the lungs is in its infancy. In particular, progress in this field has been hindered by the complex structure of the respiratory fluid and the resulting lack of understanding of the biophysical properties of the fluid. In this thesis, a series of in vitro mimetics of conducting airway mucus were developed to enable in depth studies of mucus properties and bioaerosol formation from mucus-like surfaces. These mucus mimetics overcome major limitations of currently available models by matching the primary chemical composition and key physical properties of the mimetic to that of native tracheal mucus. Three mimetics were chosen to facilitate the study of highly viscoelastic (diseased) mucus and non-diseased mucus under low shear conditions, such as breathing, or high shear conditions, such as cough. To study bioaerosol formation in vitro, an enhanced simulated cough machine (SCM) was developed to generate bioaerosols from mucus mimetic surfaces during cough. By controlling the temperature and relative humidity within the SCM, the detectability of bioaerosols generated from the mimetic surfaces was improved due to limited aerosol drying. The size distribution of the bioaerosols was multimodal, with four to five modes being observed for all surfaces probed. While varying the composition of surfactant at the air-mucus interface had a significant impact on surface viscoelastic properties, the size distribution of bioaerosols generated from these surfaces did not differ significantly. However, the ability to generate bioaerosols from different surfaces was highly dependent on surface properties of the mimetic, with highly viscoelastic surfaces generating bioaerosols in only half the experiments. This research will enhance our knowledge of bioaerosol formation in the respiratory tract and ultimately guide the development of alternative strategies to suppress bioaerosol formation.

<p> </p> <p>Interfaces separating two fluids are incredibly complex physical structures and are common throughout science, technology, and nature. Examples from daily life include the air-water interface separating a water drop that is dripping from a leaky faucet from the surrounding air and the interface of a soap bubble (which actually consists of two interfaces) separating the interior of the bubble from its exterior. Other common examples from nature include interfaces between falling rain drops and the surrounding air, and the mist that one encounters at beaches, waterfalls, and fountains where the spray droplets are separated from the surrounding air by an interface. Interfaces and manipulating them are key to technological applications such as thin film coating flows and diverse processes involving drop-by-drop processing such as ink-jet printing, drop-wise manufacturing, spray coating, DNA microarraying, and chemical separations, e.g. extraction. Aside from the coating flows example, the aforementioned situations are all examples of free surface flows that involve abrupt and catastrophic topological changes of interfaces that include physical processes such as breakup (also called pinch-off) as in drop breakup, rupture as in liquid-film or liquid-sheet rupture, and coalescence as in drop or bubble coalescence (similar phenomena also arise in sintering and/or fusion of ceramic, metallic, and polymer particles). These topological changes entail what are referred to as finite-time hydrodynamic singularities. For example, at the location(s) where a drop breaks, the thickness of the drop locally tends to zero while fluid pressure and velocity diverge (hence the reason for the word singularity). In addition to hydrodynamic singularities, the presence of surface-active agents or surfactants at fluid interfaces in free surface flows is another reason scientists have been attracted to the study of such problems.</p> <p>Adsorption onto and lowering of the surface tension of a fluid interface by surfactants are exploited in applications such as enhanced oil recovery, coating flows, lung surfactants, drop/jet breakup, and film/sheet rupture, with the latter two being among the prime motivators for this PhD thesis. However, surfactant concentration can be nonuniform at the interface because surfactant molecules can be transported along it by convection and diffusion and also due to normal dilatation and tangential stretching of the interface. Thus, aside from simply lowering surface tension, nonuniformity in surfactant concentration causes gradients in surface tension and gives rise to tangential interfacial (Marangoni) stresses. The latter brings about rich physics including tears of wine, interfacial turbulence in mass transfer, and droplet bouncing. In addition to lowering surface tension and the Marangoni effect, surfactants may also induce surface rheological or viscous effects as surfactant molecules deform against each other. The primary goal of this thesis is to advance the understanding of surface rheological effects in situations involving the breakup of surfactant-covered liquid threads (which also includes jets and drops) and liquid sheets. The fundamental understanding developed in this thesis is likely to prove indispensable in and/or assist the development of new technologies where surface rheological effects are central to the processes at hand, e.g. in controlling drop size distributions and avoiding undesirable satellite droplets and/or misting. An initially unexpected but highly rewarding outcome of the research has been the development of techniques for the measurement of surface viscosities, a task that has heretofore proven to be a formidable challenge to experimentalists.</p> <p>In this thesis, surface rheological effects in free surface flows are examined through both analytical and numerical solution of the incompressible Navier-Stokes equations subjected to the traction boundary condition augmented by the Boussinesq-Scriven constitutive equation to account for surface viscous effects. Rigorous and robust numerical algorithms based on the Galerkin finite element (GFEM) method are developed for predictions of surfactant transport, surface rheological effects and hydrodynamics in response to the motion of moving boundaries. The accuracy of computational predictions is verified by demonstrating that computed results accord well with scaling theories.</p>

Adsorption layers of soluble surfactants enable and govern a variety of phenomena in surface and colloidal sciences, such as foams. The ability of a surfactant solution to form wet foam lamellae is governed by the surface dilatational rheology. Only systems having a non-vanishing imaginary part in their surface dilatational modulus, E, are able to form wet foams. The aim of this thesis is to illuminate the dissipative processes that give rise to the imaginary part of the modulus. <br><br> There are two controversial models discussed in the literature. The reorientation model assumes that the surfactants adsorb in two distinct states, differing in their orientation. This model is able to describe the frequency dependence of the modulus E. However, it assumes reorientation dynamics in the millisecond time regime. In order to assess this model, we designed a SHG pump-probe experiment that addresses the orientation dynamics. Results obtained reveal that the orientation dynamics occur in the picosecond time regime, being in strong contradiction with the two states model. <br><br> The second model regards the interface as an interphase. The adsorption layer consists of a topmost monolayer and an adjacent sublayer. The dissipative process is due to the molecular exchange between both layers. The assessment of this model required the design of an experiment that discriminates between the surface compositional term and the sublayer contribution. Such an experiment has been successfully designed and results on elastic and viscoelastic surfactant provided evidence for the correctness of the model. <br><br> Because of its inherent surface specificity, surface SHG is a powerful analytical tool that can be used to gain information on molecular dynamics and reorganization of soluble surfactants. They are central elements of both experiments. However, they impose several structural elements of the model system. During the course of this thesis, a proper model system has been identified and characterized. The combination of several linear and nonlinear optical techniques, allowed for a detailed picture of the interfacial architecture of these surfactants. / Amphiphile vereinen zwei gegensätzliche Strukturelemente in einem Molekül, eine hydrophile Kopfgruppe und ein hydrophobe, meist aliphatische Kette. Aufgrund der molekularen Asymmetrie erfolgt eine spontane Adsorption an der Wasser-Luft Grenzfläche. Die Adsorptionsschicht verändert die makroskopischen Eigenschaften des Materials, z.B. die Grenzflächenspannung wird erniedrigt. Amphiphile sind zentrale Bauelemente der Kolloid- und Grenzflächenforschung, die Phänomene, wie Schäume ermöglichen. <br><br> Eine Schaumlamelle besteht aus einem dünnen Wasserfilm, der durch zwei Adsorptionsschichten stabilisiert wird. Die Stabilität der Lamelle wird durch die Grenzflächenrheologie entscheidend geprägt. Die wesentliche makroskopische Größe in diesem Zusammenhang ist das so genannte Grenzflächendilatationsmodul E. Es beschreibt die Fähigkeit des Systems die Gleichgewichtsgrenzflächenspannung nach einer Expansion oder Dilatation der Adsorptionschicht wieder herzustellen. Das Modul E ist eine komplexe Größe, in dem der Imaginärteil direkt mit der Schaumstabilität korreliert. <br><br> Diese Arbeit widmet sich der Grenzflächenrheologie. In der Literatur werden zwei kontroverse Modelle zur Interpretation dieser Größe diskutiert. Diese Modelle werden experimentell in dieser Arbeit überprüft. Dies erfordert die Entwicklung neuer experimenteller Aufbauten basierend auf nichtlinearen, optischen Techniken. Mit diesen Experimenten konnte eines der Modelle bestätigt werden.

Dans les travaux de recherche développés durant cette thèse, une première approche desécoulements magnétohydrodynamiques (MHD) multiphasiques est proposée. Cette approche seconcentre sur les phénomènes liés à l’interaction entre une dynamique interfaciale et un écoulementde coeur MHD. Le couplage induit entre rhéologie de surface etMHDde sous-phase est particulièrementillustré par le développement d’un viscosimètre annulaire surfacique, dédié à l’étude desmétaux liquides progressivement oxydés. En premier lieu sont introduits les éléments théoriquespropres à laMHDet à la rhéologie de surface. La modélisation de leur couplage fait intervenir deuxparamètres interfaciaux : les viscosités surfaciques dilatationnelle et de cisaillement. L’influence respectivede ces deux paramètres sur l’écoulement MHD de sous-phase est étudiée analytiquementet numériquement dans le cas d’un écoulement (stratifié) annulaire MHD permanent. Dans la configurationretenue, un champ magnétique uniforme vertical est imposé, perpendiculairement à lasurface liquide graduellement oxydée. Le rôle décisif des contraintes visqueuses interfaciales concernantl’(in)activation des couches de Hartmann est démontré, conduisant à des topologies atypiquesd’écoulement MHD. Le viscosimètre annulaire MHD est ensuite proposé en tant que méthodeexpérimentale originale, permettant la mesure sélective des viscosités surfaciques de fluides électroconducteurs.Les premières campagnes expérimentales aboutissent à une estimation de la viscositéde cisaillement interfacial d’un alliage métallique (GaInSn) liquide à température ambiante. Finalement,une ouverture sur l’écoulement MHD à proximité d’une inclusion gazeuse sphérique rigideest discutée en annexe de ce projet, en lien avec des conditions mécaniques variables à l’interfaceliquide/gaz pilotées par la rhéologie de surface, constituant une première approche vers la descriptiondes écoulements MHD dispersés. / In this thesis work, a first approach towards the description of magnetohydrodynamic(MHD) multiphase flows is proposed, based on the investigation of the role of surface rheologyin permanent regime. The study of the coupling between bulk MHD and surface rheology is particularlymotivated by the development of an annular surface viscometer devoted to liquid metalstopped with an oxidation layer. First, theoretical foundations of MHD and of surface rheologyare separately introduced. The modelling brings out a strong coupling between bulk and surfacevelocities, the latter being dependent on two interfacial parameters: the surface shear and dilatationalviscosities. Their respective influence is analytically and numerically investigated in the caseof a permanent annular (stratified) MHD end-driven flow. In the considered geometry, a vertical(uniform) magnetic field is imposed, perpendicular to the gradually oxidising liquid surface. Thecontribution of planar surface viscous stresses to the possible electrical activation of Hartmannlayers is demonstrated, leading to a variety of atypical MHD flow patterns. The annular MHDviscometer is then developed as a first device able to perform selective measurement of the surfaceviscosities of electroconductive fluids. First experiments lead to an estimated value of the surfaceshear viscosity for a liquid alloy (GaInSn) at room temperature. Some hints are finally given to investigatethe study case of aMHDflow past a rigid fluid sphere, with varying interfacial conditionsgoverned by surface rheology, as an additionalwork constituting a first step towards the descriptionof dispersed MHD flows.