As drop-on-demand (DOD) applications continue to gain ground in desktop inkjet-printing, 3D printing, fluid mixing, and other areas the demand for higher frequency operations are beginning to push against the current physical boundaries in DOD technology. The current research is exploring the possibility of controlling drop volume and velocity at high frequency ranges where meniscus vibrations can occur between drop formations and affect drop formation characteristics. A periodic voltage is applied to a piezoelectric disk in order to generate pressure fluctuations in a single nozzle droplet generator, causing the fluid meniscus at the nozzle to vibrate. A single stronger pulse is then superimposed over the periodic waveform at different phases in order to drive drop ejection. The characteristics of the resulting drop, specifically the volume and velocity, are experimentally measured using a high speed camera with precise timing control. The results of these experiments are then compared to a lumped element model (LEM) developed for the droplet generator geometry used. Within the LEM model framework, special attention was given to the definition of a novel method by which one can measure drop volume within an electroacoustic circuit and also allow meniscus dynamics to affect present and future drop formations. Experimental results indicate a strong dependence of both drop volume and drop velocity on the phase of the vibrating meniscus at the start of drop formation. Positive meniscus displacements and momentums resulted in large drop volumes and velocities while negative displacements could reduce drop volume or altogether eliminate drop formation. Specifically, positive displacements and momentum of a vibrating meniscus could lead to drop volumes approximately 50% larger than the original drop volume without a vibrating meniscus. Meanwhile, negative meniscus displacements and momentums were shown to have the ability to completely prevent drop formation. Additional potential for drop characteristic control with a vibrating meniscus is discussed alongside observations on the stabilizing affect the vibrating meniscus appears to have on drop velocity as a function of time. Also, flow visualization of the drop formation is provided to demonstrate the added affect the meniscus vibrations have on the drop shapes and break-off profiles. The LEM model presented demonstrates qualitative agreement with the experimental model, but fails to quantitatively predict drop volumes. Sources of error for the LEM model and potential improvements are discussed. / Graduation date: 2012

The word piezo in greek means \to compress". Piezoelectric sensors work on the principle of direct piezoelectric effect, where a mechanical input generates a corresponding electric charge. The advantages of these sensors are wide fre-quency range of operation, high stiffness and small size. The main limitation of a piezoelectric sensor is that it cannot be used in measurements that are truly static. When a piezoelectric sensor is subjected to a static force, a fixed amount of charge is developed which would eventually decay at a rate dependent on the external impedance of the sensor circuitry. Operating sensors at resonance have been one of the methods to overcome the limitation of using piezoelectric sensors for static measurements. However, since both actuation and sensing are done by the same piezoelectric element, this results in a cross-talk of input and output signals. The drawback of using single piezoelectric element for actuation and sensing is overcome in this work by using two identical elements|one for actuation and one for sensing. The operating frequency is about 10 % of the natural frequency of the sensor, thus enabling to operate the sensor in non resonant mode. Since the actuation and sensing mechanisms are separated, static measurement can be carried out. The output signal from the sensing element is monitored by a Lock-in amplifier which works on the principle of phase sensitive detection. The advantage of this sensor design is high sensitivity along with narrow band detection. It can be shown that the voltage output of the sensor Vout / a1 + m(b1 + b2F + b3K) + c1F + d1K, where m and K are the external mass and interaction stiffness, respectively, F is the force acting on it. By maintaining any two of these three quantities constant, the remaining one can be measured without any difficulty. The non resonant mode of operation makes it possible to explore the potential of this sensor in investigating mechanics of solid-liquid (viscous), solid-solid (inelastic) and solid-tissue(viscoelastic) interactions. High sensitivity, wide range of measurement (1 g{1 g) and high resolutio(0.1 g) of the non resonant mass sensor makes it possible to use it in measure-ment of very small masses of the order 1 g. Typically, resonant sensors such as quartz crystal microbalance (QCM) are used for mass measurements at that range. However, since the performance of resonant sensors is controlled by damp-ing, a phenomenon known as `missing mass effect' arises. Operating a sensor in non resonant mode (stiffness controlled mode) is a way to overcome this problem, especially when the mass is viscous and/or viscoelastic in nature. Drosophila fly, egg and larvae are the viscoelastic masses that are measured using this non res-onant sensor. Evaporating sessile drops of water and Cetyl trimethylammonium bromide (CTAB) surfactant solution from nominally flat surfaces are monitored to characterize the sensor for viscous mass measurement. Evaporation rate per unit surface area remains more or less constant, during the initial stages of evap-oration. When the surfactant concentration is varied, evaporation rate per unit surface area is highest for solutions around critical miscelle concentration (CMC). A study is carried out to understand the effect of concentrations on spreading of ink over inkjet printing paper. It is found that the spreading is least around CMC, since spreading is dependent on the rate of evaporation. The non resonant piezoelectric sensor which has high stiffness and quick re-sponse is also capable of measuring very small frictional forces. This sensor is configured to work as an inertial slider. Friction measurement at micro scales is important for designing microsystems such as stick-slip actuators. At such length scales, experiments have to performed at low loads and high excitation frequencies. The support stiffness of such systems should be high and the force of friction generated during slipping, when displacements are smaller than the contact radius, are of the order of few N. The displacement during slipping (S) is dependent on the amplitude of the input voltage to the actuation element. The frictional force measured during slipping by the sensor element indicates that the co-efficient of friction ( ) is independent of the sliding velocity. The developed non resonant sensor in this work under small amplitude exci-tation, can measure force gradient (i.e. stiffness). The total force generated when a needle is inserted into a viscoelastic material is a sum of force due to stiffness of the material, friction and the cutting force at the tip. The force due to stiffness is dominant when the needle is bending the tissue before the puncture occurs. Use of the non resonant sensor in tandem with strain gauge force sensor enables distinguishing the three components of the total force. The slope of the force-displacement (F -d) curve during the initial stages of needle penetration into the viscoelastic material, before puncture, is indicative of the stiffness of the mate-rial. The peak force measured during penetration is higher for needles with larger diameters and lower insertion velocities. The viscoelastic response (relaxation) of the material remains independent of the insertion velocity, for a given thickness of the material and a constant needle diameter. In summary, the sensor designed and developed in this work operates in stiffness controlled mode to eliminate the `missing mass effect' encountered dur-ing resonant mode of operation, has been clearly highlighted. Mass, force and stiffness measurements are possible over a wide range just by varying the ampli-tude of the input signal to the actuator element. The advantages such as high stiffness, small size and high response makes it advantageous to carry out in-situ micro scale studies in scanning electron microscopy (SEM) and transmission electron microscopy (TEM).

Ce travail de thèse porte sur le développement technologique d’outils miniaturiséspour l’exploration de diagrammes de phase de fluides complexes (dispersions colloïdales,solutions de polymères ou tensioactifs, etc). Les outils élaborés permettent dedéterminer des diagrammes de phase par une approche continue à l’aide de la microfluidique.Ils sont basés sur deux types de procédés membranaires différents : la pervaporation(mécanisme d’évaporation de solvant) et la dialyse (mécanisme d’échangesosmotiques). En s’appuyant sur le processus de pervaporation, il a été montré théoriquementet expérimentalement qu’il existe une géométrie pour laquelle le séchageconfiné est homogène. Il est donc possible de construire des diagrammes de phase demélanges à plusieurs composants de l’échelle moléculaire aux colloïdes. Une étudeconsacrée à la compréhension de la complexité du séchage des nanoparticules de silicecommerciales dans un canal microfluidique de type microévaporateur a été miseen place. La cinétique de concentration des particules est décrite jusqu’à la formationd’un état dense ainsi que les divers phénomènes liés au séchage comme l’existenced’une transition de phase dans un système colloïdal, l’apparition de fractures ou la délaminationdu matériau dense. Un nouvel outil microfluidique intégrant une membranede type dialyse offre la possibilité de contrôler les échanges osmotiques à l’échelle dunanolitre. Le protocole de fabrication ainsi que le dimensionnement de la géométriesont présentés. Grâce à cet outil, il est possible de mesurer des pressions osmotiquesde dispersions colloïdales. / This work deals with the technological development of miniaturized tools for theexploration of the phase diagram of complex fluids (colloidal dispersions, solutions ofpolymers or surfactants, etc). The microfluidic tools we elaborated make it possibleto determine phase diagrams of a series of formulations of complex fluids by consumingonly minute amounts of samples. These devices exploit two types of membraneprocesses to concentrate the chemical species : pervaporation (solvent evaporationthrough a dense membrane) and dialysis (osmotic exchanges through a membrane).Concerning the case of pervaporation, we demonstrated theoretically and experimentallythat a specific microfluidic design exists for which concentration fields of chemicalspecies remain spatially homogeneous along the kinetic path followed withinthe phase diagram. Then, it enables to obtain phase diagrams of multi-componentsmixtures from molecular compounds up to colloids, at the nanolitre scale. We reporta study concerning the understanding of the drying process of commercial silica nanoparticlesusing a dedicated microfluidic experiment involving pervaporation. Wepresent the kinetics of the concentration of the particles within the channel up to theformation of a dense colloidal packed bed which invades the channel at a controlledrate. We developed an original microfluidic tool integrating a dialysis membranewhich makes it possible to control osmotic exchanges at the nanoliter scale. We reportthe protocol of microfabrication of this chip and its specific geometry.We presentpreliminary results showing that this tool can be used to measure osmotic pressures ofcolloidal suspensions.

Lors d’un accident grave dans un réacteur nucléaire (REP ou REB en particulier), le combustible fondu (corium) peut se déverser dans le réfrigérant (eau). L’interaction entre les deux fluides est appelée Interaction Combustible-Réfrigérant. Sous certaines conditions, cette interaction peut conduire à une «explosion de vapeur» qui peut menacer le confinement du réacteur nucléaire. L’ICR est une interaction de caractère multiphasique complexe où divers phénomènes physiques interviennent de manières couplées. Elle débute par une phase de mélange entre les fluides (prémélange), se traduisant par la fragmentation du corium et sa dispersion dans le réfrigérant. Ce processus de fragmentation impacte les échanges thermiques (ébullition et mise en mouvement du fluide environnant (réfrigérant)) et les processus chimiques (oxydation du corium et génération d’hydrogène). Cette thèse apporte de nouveaux éléments concernant la compréhension physique et la modélisation du phénomène de fragmentation du corium, dont l’objectif principal est d’améliorer la modélisation dans le logiciel de thermohydraulique multiphasique MC3D, développé par l’IRSN. L’étude proposée se base sur l’hypothèse de la modélisation de la fragmentation comme un phénomène multi-échelle avec un découplage entre taux de fragmentation du jet et dimension des gouttes résultantes. Elle suppose un processus de fragmentation qui est le résultat d’une déstabilisation primaire (passage jet -> grosses gouttes) pilotée par les grandes échelles de l’écoulement et d’un processus de déstabilisation secondaire menant à une fragmentation finale dépendante des paramètres plus «locaux» de l’écoulement. Nous avons conjugué notre modélisation avec une méthode de type MUSIG récemment introduite dans le logiciel MC3D. Les gouttes de corium y sont représentées, via un découpage en classes, par plusieurs champs de masse et d’énergie avec des diamètres distincts. Malgré les avancées dans la modélisation de la fragmentation, la compréhension des mécanismes et la caractérisation de la fragmentation des gouttes liquides est encore très imparfaite, particulièrement dans le cas liquide/liquide. Le travail de thèse s’est alors orienté vers l’analyse de ce processus en utilisant le logiciel de simulation GERRIS. L’étude conduit à proposer une nouvelle carte de régimes de fragmentation en configuration liquide/liquide, une compréhension plus approfondie de la dynamique de fragmentation et une analyse sur l’interaction vortex-goutte pilotant la transition entre les régimes. / In the case of a severe accident in a nuclear power plant, the molten core may flow into water and interact with it. The consequences of this fuel-coolant interaction (FCI) for the follow-up of the accident may be numerous so the phenomenon needs to be described accurately, one of them called “steam explosion” can lead to the failure of the nuclear reactor containment. FCI is a complex multiphase interaction involving several physical phenomena. The premixing phase of the interaction consists in the fragmentation and dispersion of corium in the coolant pool. This phase is driven by the fragmentation process which modifies heat transfers (coolant boiling dynamics) and chemical reactions (corium oxidation and hydrogen generation). This thesis brings new elements about the corium jet and droplet breakup with the main goal of improve fragmentation models on the MC3D multiphase code, developed by the IRSN. Our study is based on a multi-scale fragmentation process where the jet fragmentation rate and final droplet dimensions are not coupled themselves. We suppose a fragmentation process resulting from a primary instability (mass transfer within jet and big droplets) depending on the large flow scales and a secondary instability depending on the small flow scales (leading to final droplet breakup). This model has been implemented in MC3D in combination with the MUSIG method recently added to MC3D. In this method, droplets are represented using several classes, each of them with their own droplet diameter, mass and energy fields. Despite new improvements on modeling corium fragmentation, there is still a lack on the comprehension and characterization on the liquid droplet fragmentation, particularly on liquid/liquid configurations. In this thesis, we study in detail droplet breakup using the computational fluid dynamics software GERRIS. As a result, we find a new droplet breakup classification in liquid/liquid configurations, we improve the droplet breakup dynamics comprehension and we analyze the droplet-vortex interaction to determine breakup regime transition.

L'évaporation d'une goutte reposant sur un support plat semble être un système relativement simple à étudier et a fait l'objet d'études scientifiques depuis plus d'un siècle. Cependant, l'étude de l'évaporation de gouttes sessiles est toujours d'actualité aujourd'hui avec l'essor de nouvelles techniques de visualisation ou de l'apparition de nouveaux types de fluides complexes.Cette étude expérimentale sera focalisée sur deux aspects distincts :- L'étude sur l'évaporation de fluides purs permettra d'étudier la dynamique d'évaporation et les ondes hydrothermales qui apparaissent dans les gouttes de fluides volatils lors du changement de phase. L'influence du type de fluide (différents alcools et alcanes) et du niveau de gravité (terrestre, lunaire et martienne) seront étudiés. De plus, l'utilisation de différents niveaux de gravité permet de développer un modèle empirique afin de prendre en compte dans le modèle quasi-stationnaire limité par diffusion de la vapeur la convection naturelle qui augmente fortement le débit d'évaporation.- Si les fluides complexes présentent une dynamique de séchage similaire à celle des fluides purs, d'autres mécanismes entrent en jeux, comme la gélification, l'organisation des particules et l'apparition de craquelures (voir Figure 2). Le mouillage et les différents groupes fonctionnels graphés sur les particules seront étudiés en regard du motif final de craquelures. / Sessile droplets are widely found in day to day life: it might be a coffee spilt, rain onto a waterproof raincoat or again, water falling onto a cooking plate. However, despite the vast number of studies devoted to droplets for almost half a century, the fundamental phenomenon of the evaporation of sessile droplets is still a field that attracts a high level of interest due to its wide applicability and the development of new visualisation techniques or new types of complex fluids. This experimental study is focused two distinct aspects:- The evaporation of pure fluids has allow to study hydrothermal waves that appear in the droplets of volatile fluids during phase change. The influence of the type of fluid ---different alcohols and alkanes--- and the gravity levels ---Terrestrial, Lunar and Martian--- is investigated to have a better understanding of the flow motion inside droplet. Moreover, the use of different gravity levels allows to experimentally evidence the contribution of the atmospheric convective transport to sessile droplet evaporation. This investigation has allowed to develop an empirical model to take account of natural convection which greatly increases the evaporation rate in the quasi-steady diffusion-controlled evaporation model.- If complex fluids exhibit an evaporation dynamic similar to pure fluid, other mechanisms come into play, such as gelation, particles organisation and cracks formation. Wetting and different functional groups on the particles graphs will be studied in relation to the final pattern of cracks.

Modifying eye drops using hyaluronan leads to an increased retention time on the eye surface. Long-lasting observations of the stability of two different eye drops, Opthalmo-Septonex and Visine Classic, after the addition of hyaluronan with varying concentration are presented in this work. The interactions of hyaluronan with the eye drops, or their components benzalkonium chloride and tetryzoline, are investigated by monitoring particle sizes and the charge of the molecules. Additionally, rheological examinations of the samples are done and the mucoadhesion index is determined by using the mucine method.

The design of fluid management systems requires accurate models for fluid transport. In the low gravity environment of space, gravity no longer dominates fluid displacement; instead capillary forces often govern flow. This thesis considers the redistribution of fluid along an interior corner. Following a rapid reduction of gravity, fluid advances along the corner measured by the column length z = L(t), which is governed by a nonlinear partial differential equation with dynamical boundary conditions. Three flow types are examined: capillary rise, spreading drop, and tapered corner. The spreading drop regime is shown to exhibit column length growth L ~ t2/5, where a closed form analytic solution exists. No analytic solution is available for the capillary rise problem. However, a perturbed power law similarity solution is pursued to approximate an analytic solution in the near neighborhood of the exact solution for the spreading drop. It is recovered that L ~ t1/2 for the capillary rise problem. The tapered corner problem is not analytically understood and hence its corresponding L is undocumented. Based on the slender corner geometry, it is natural to hypothesize the tapered corner column length initially behaves like the capillary rise regime, but after sufficient time has elapsed, it transitions into the spreading drop regime. This leads to a conjecture that its column length growth L is restricted to t2/5 < L < t1/2. To verify this conjecture an explicit finite difference numerical solution is developed for all three regimes. As will be shown, the finite difference scheme converges towards the analytic solutions for the spreading drop and capillary rise regimes. From this we assume the finite difference scheme is accurate for corner flows of similar geometries, and thus apply this scheme the more onerous criteria of the tapered corner. Numerical results support the conjectured L behavior for the tapered corner. Understanding the dynamics of such flows and responses to various geometries offers design advantages for spacecraft waste-management systems, fuel control, hydration containment, cryogenic flows, and a myriad of other fluid applications.

This dissertation deals with instabilities of thin liquid films up to entrainment of drops. Four types of instabilities have been classified depending on the type of structure and process on the liquid film surface: two-dimensional slow waves, two-dimensional fast waves, three-dimensional waves, solitary waves and entrainment of drops from the film surface. This thesis analyzes the physical principles of instabilities and deals with the mathematical formulation of the problem. Shear and pressure forces acting on the surface of the liquid film are identified as the cause of instabilities. Mathematical models for predicting instabilities are demonstrated using approaches based on solving the Orr-Sommerfeld equation and the equations of motion in integral form. Models of shear and pressure forces acting on the surface of the film and selected models of film thickness are presented. The work is focused on the prediction of the initiation of two-dimensional waves using the integral approach. Shear stress and pressure forces acting on the liquid film surface have been modeled using the simulation of air flow over a solid surface. Finally, criteria for drop entrainment are presented with their dependence on air velocity and film thickness.

Seit mehr als einem Jahrhundert ist ein wachsendes wissenschaftliches Interesse an Tropfen und den Vorgängen bei deren Aufprall auf die verschiedensten Substrate zu verzeichnen, wohl auch durch die Fotografien von Worthington (1908) ausgelöst. Inzwischen wurden viele Erkenntnisse durch große Fortschritte bei der experimentellen Untersuchung (z.B. mittels Hochgeschwindigkeitsaufnahmen) und durch theoretische und computergestützte Untersuchung (z.B. durch skalenfreie und numerische Modellierung) gewonnen. Trotzdem bleibt durch die Vielfältigkeit und Komplexität der Phänomene während des Tropfenaufpralls sowie wegen der ständig erweiterten Anwendungsbereiche dieses Forschungsgebiet hochaktuell. Insbesondere sehr kleine und gleichzeitig sehr schnelle Tropfen (Tropfendurchmesser 10µm bis 100µm, Tropfengeschwindigkeit 10m/s bis 100m/s) kommen in vielen modernen Anwendungen vor (z.B. Verbrennungsmotoren, Tintenstrahldrucker, Reinigung von Oberflächen). In diesem wichtigen, aber für Untersuchungen schwer zugänglichen Parameterbereich gibt es immer noch offene Fragen. Die vorliegende Arbeit beschäftigt sich daher mit diesen schnellen Mikrotropfen in Bezug auf ihre Herstellung und den Aufprallvorgang auf ein festes, trockenes oder benetztes Substrat. Zunächst wird eine Methode zur Erzeugung eines Hochgeschwindigkeitssprays realisiert, welche auf dem durch Ultraschall gesteuerten Plateau-Rayleigh-Zerfall eines Flüssigkeitsstrahls beruht. Sie ermöglicht es, sowohl Tropfengröße als auch –geschwindigkeit präzise und mit hoher Reproduzierbarkeit über den gesamten oben angegebenen Parameterbereich einzustellen. Durch gezielte Manipulation eines Einzeltropfens durch elektrische Felder wird anschließend der Tropfenaufprall auf Substrate unterschiedlicher Benetzbarkeit mit sehr hoher zeitlicher Auflösung (ca. 100 Mio. Bilder pro Sekunde) bei gleichzeitig hoher räumlicher Auflösung (< 1µm) untersucht. Es zeigt sich, dass bekannte Modelle für langsamere und größere Tropfen im Millimeterbereich auch für schnelle Mikrotropfen Gültigkeit behalten. Somit ist bei gleichen dimensionslosen Kennzahlen (z.B. Reynolds-Zahl, Weber-Zahl, Ohnesorge-Zahl) eine skalenfreie Beschreibung des Tropfenaufpralls möglich. Schließlich wird die Methode zur Tropfenerzeugung auf einen für Anwendungen in der Reinigung relevanten Fall übertragen. Hierbei geht es um den Tropfenaufprall auf ein von einem Flüssigkeitsfilm überströmten Substrat. Es werden die während des Auftreffvorgangs auftretenden Geschwindigkeiten in der sich bildenden radialen Strömung in Abhängigkeit von verschiedenen Prozessparametern bestimmt. Aus den Ergebnissen lassen sich Aussagen über die zu erwartende Reinigungswirkung durch derartige Tropfen und den Einfluss der Prozessparameter treffen.

L’objectif de cette thèse consiste à déterminer l’influence d’une pression ambiante comprise entre 100 à 600 KPa sur l’évaporation d’une goutte, puis sur l’évaporation d’un spray soumis aux mêmes conditions. La première étape consiste à étudier l’influence de la pression ambiante sur l’évolution de la forme, du diamètre, de la vitesse et du débit d’évaporation d’une goutte de liquide en chute libre. Pour cela, une technique de mesure optique a été utilisée et une méthodologie a été développée pour calibrer cette technique de mesure et ainsi minimiser les erreurs de mesures sur la taille des particules. En parallèle, un modèle analytique d’évaporation de gouttes en chute libre a été développé : une attention particulière a été portée sur la détermination d’une corrélation adaptée au calcul du coefficient de traînée afin de tenir compte de l’évolution de la forme des gouttes au cours de leur chute. Ce modèle d’évaporation de gouttes est comparé à un modèle d’évaporation de spray (prenant en compte l’entrainement d’air, la concentration de vapeur au loin de la goutte et l’influence de la pression ambiante) pour montrer les limites du modèle d’évaporation de gouttes lors de son application à l’évaporation d’un spray. La deuxième étape de l’étude a consisté à appliquer les techniques de mesure et d’analyse mises au point précédemment à l’étude de la granulométrie d’un spray pour caractériser l’influence de trois paramètres : la pression ambiante, la pression d’injection du liquide et la nature du liquide. L’analyse des résultats a permis de développer un modèle statistique pour déterminer la granulométrie de ces sprays. / The objective of this thesis is to determine the influence of ambient pressure between 100 and 600 KPa on the evaporation of a drop, and on the evaporation of a spray in the same conditions. The first step is to study the influence of ambient pressure on the evolution of the shape, the diameter, the speed and the evaporation rate of a drop of liquid in free fall. Then, an optical measurement technique has been used and a methodology was developed to calibrate this measurement technique and minimize measurement errors on the particle size. In parallel, an analytical model of evaporation of falling drops has been developed: a particular attention was paid to the determination of an appropriate correlation for the drag coefficient to take into account changes in the shape of drops during their fall. This model of evaporation of drop is compared with a spray evaporation model (taking into account the training of air, the vapor concentration away form the drop and the influence of the pressure to show the limits of this drop evaporation model when applied to the evaporation of a spray. The second phase of the study was to apply the measurement techniques and analysis developed previously to study the drop size of a spray to characterize the influence of three parameters: ambient pressure, injection pressure of the liquid and nature of the liquid. The analysis of the results allowed developing a statistical model to determine the size of the drops of these sprays.