Droplet evaporation is ubiquitous to multitude of applications such as microfluidics, surface patterning and ink-jet printing. In many of the process like food processing tiny concentrations of suspended particles may alter the behavior of an evaporating droplet remarkably, leading to partially viscous and partially elastic dynamical characteristics. This, in turn, may lead to some striking mechanical instabilities, such as buckling and rupture. In this thesis, we provide a comprehensive physical description of the vaporization, self-assembly, agglomeration and buckling kinetics of sessile nanofluid droplet pinned on a hydrophobic substrate in various configurations. We have deciphered five distinct regimes of droplet lifecycle. Regime I-III consists of evaporation induced preferential agglomeration that leads to the formation of unique dome shaped inhomogeneous shell with stratified varying density liquid core. Regime IV involves capillary pressure initiated shell buckling and stress induced shell rupture. Regime V marks rupture induced cavity inception and growth. We provide a regime map explaining the droplet morphology and buckling characteristics for droplets evaporating on various substrates. Specifically, we find that final droplet volume and radius of curvature at buckling onset are universal functions of particle concentration. Furthermore, flow characteristics inside the heated and unheated droplets are investigated and found to be driven by the buoyancy effects. Velocity magnitudes are observed to increase by an order at higher temperatures with self-similar flow profiles. With an increase in the surface temperature, droplets exhibit buckling from multiple sites over a larger sector in the top half of the droplet. In addition, irrespective of the initial nanoparticle concentration and substrate temperature, hydrophobicity and roughness, growth of daughter cavity (subsequent to buckling) inside the droplet is found to be controlled by the solvent evaporation rate from the droplet periphery. The results are of great significance to a plethora of applications like DNA deposition and nanofabrication. In the next part of the thesis, we deploy the droplet in a rectangular channel. The rich physics governing the universality in the underlying dynamics remains grossly elusive. Here, we bring out hitherto unexplored universal features of the evaporation dynamics of a sessile droplet entrapped in a 3D confined fluidic environment. Increment in channel length delays the completion of the evaporation process and leads to unique spatio-temporal evaporation flux and internal flow. We show, through extensive set of experiments and theoretical formulations, that the evaporationtimescale for such a droplet can be represented by a unique function of the initial conditions. Moreover, using same theoretical considerations, we are able to trace and universally merge the volume evolution history of the droplets along with evaporation lifetimes, irrespective of the extent of confinement. These results are explained in the light of increase in vapor concentration inside the channel due to greater accumulation of water vapor on account of increased channel length. We have formulated a theoretical framework which introduces two key parameters namely an enhanced concentration of the vapor field in the vicinity of the confined droplet and a corresponding accumulation lengthscale over which the accumulated vapor relaxes to the ambient concentration. Lastly, we report the effect of confinement on particle agglomeration and buckling dynamics. Compared to unconfined scenario, we report non-intuitive suppression of rupturing beyond a critical confinement. We attribute this to confinement-induced dramatic alteration in the evaporating flux, leading to distinctive spatio-temporal characteristics of the internal flow leading to preferential particle transport and subsequent morphological transitions. We present a regime map quantifying buckling & non-buckling pathways. These results may turn out to be of profound importance towards achieving desired morphological features of a colloidal droplet, by aptly tuning the confinement space, initial particle concentration, as well as the initial droplet volume. These findings may have implications in designing functionalized droplet evaporation devices for emerging engineering and biomedical applications.

The study presented in this dissertation concerns the evaporation, in normal ambient conditions, of sessile droplets (pinned and freely receding) of various HFE liquids (instead of the widely used water), which are considered so far as environmentally friendly and are often used as heat-transfer fluids in thermal management applications. They are pure perfectly-wetting and volatile liquids with low thermal conductivity and high vapor density. These properties affect in their own way many aspects concerning droplet evaporation such as the evaporation-induced contact angles, evaporation rate of a droplet, contact line pinning and Marangoni flow, all of which are treated in the present dissertation.<p>In general, the thesis starts with a general introduction including but not limited to sessile droplets (Chapter 1). In Chapter 2 we provide a general overview of capillarity-related concepts. Then, in Chapter 3 we present the interferometric setup, along with the liquids and the substrate that is used in the experiments, and also explain the reasons why this particular method is chosen. In Chapter 4 we address, among others, the issue of evaporation-induced contact angles under complete wetting conditions. The behavior of the global evaporation rate is also examined here, whereas in Chapter 5 we discuss the influence of thermocapillary stresses on the shape of strongly evaporating droplets. Finally, before concluding in Chapter 7, we address in Chapter 6 the still open question of the influence of non-equilibrium effects, such as evaporation, on the contact-line pinning at a sharp edge, a phenomenon usually described in the framework of equilibrium thermodynamics. The experimental results obtained are also compared with the predictions of existing theoretical models giving rise to interesting conclusions and promising perspectives for future research.<p> / Doctorat en Sciences de l'ingénieur / info:eu-repo/semantics/nonPublished

The first step on the way to understanding the complicated dynamics of spray is to study the behavior of isolated droplets. In many industrial and natural processes such as turbulent combustion, agricultural sprays, spray cooler, falling raindrops and cloud evolution the droplet is subjected to a chaotic unsteady external flow field. The interaction between the liquid and gaseous phases results in very intricate droplet dynamics like capillary instabilities, atomization, droplet collision and coalescence and vaporization, to name a few. In this dissertation, the focus is on shape oscillations, atomization and vaporization dynamics of pendant and sessile droplets. A droplet residing on a substrate which vibrates vertically at ultrasonic frequency will exhibit different modes of shape oscillation. The competition between capillary forces and inertia forces is basically responsible for these oscillations. However, when an acoustic force field is introduced asymmetrically around the droplet, we discover with the help of ultra high-speed imaging, a new droplet spreading phase. This new method of droplet manipulation could nd application in micro fluidics and lab-on-a-chip systems. By lading the droplet with nanoparticles, the spreading rate can be easily controlled. The spreading phase is followed by an atomization phase where surface ligaments grow to disintegrate into daughter droplets; the intensity of atomization is found to decrease with increase in fluid viscosity. The ability to control atomization characteristics of droplets by lading them with nanoparticles is a powerful technique that may be implemented in spray coolers and combustors to control the spray characteristics or combustion efficiency. Both the spreading and ligament dynamics have been theoretically simulated and the physics behind the observed trends is explained. The growth rate of the ligaments is found to be governed by Weber number modified to include the acoustic pressure level of the standing wave. The frequency of ligament breakup is found to decrease with fluid viscosity and this observation is adequately supported by a theory developed based on the evolution crater on the droplet surface. Turning now to the pendant droplets, by decomposing the droplet shape into Legendre modes, the shape oscillations exhibited by a droplet hanging from the junction of cross-wire placed at the center of an air jet is studied. Both high-speed imaging and hot-wire anemometry are employed. The driving force of oscillation of droplets subjected to the air jet is proved to be the inherent pressure fluctuations in the jet. The effect of surface tension, viscosity and Reynolds number on the shape oscillation level has been examined. The first experimental evidence of viscous attenuation of lower frequencies in a particular mode in glycerol/water mixture is reported. A theoretical model was developed to simulate the droplet shape oscillations induced by different ambient flow fields like pulsatile flow, vortical flow and flow with broadband energy spectrum. The time of interaction of the droplet with an eddy in the flow is found to be very crucial in determining the amplitude of oscillation of the droplet. The shorter the interaction time, the higher are the chances of the droplet oscillation being pushed into resonance. Finally, the heat transfer and droplet regression dynamics of pendant droplets in a hot air stream of various chemical compositions (like conventional fuels, alternative fuels and nanosuspensions) have been experimentally analyzed using high speed imaging. The droplet is deployed at the junction of cross-wire at the centre of a vertical air jet. A hybrid timescale has been proposed which incorporates the effects of latent heat of vaporization, saturation vapor pressure and thermal diffusivity. This timescale in essence encapsulates the different parameters that influence the droplet vaporization rate. The analysis further permitted the evaluation of the effect of various parameters such as surrounding temperature, Reynolds number, far-field vapor presence, impurity content and agglomeration dynamics (nanosuspensions) in the droplet.

Experimental vibration analysis of mechanical structures is a well established field.Plenty of literature exists on macro scale structures in the fields of civil, mechanical and aerospace engineering, but the study of vibrations of micro scale structures such as MEMS, liquid droplets, and biological cells is relatively new. For such structures, the amplitudes of vibration are typically in nanometeror sub-nanometer range and the frequencies are in KHz to MHz range depending upon the dimensions of the structure. In our study, we use a scanningLaser Doppler Vibrometer (LDV) to measure the vibrations of micro-scale objects such as MEMS structures, micro droplets and cells. The vibrometercan capture frequency response up to 24 MHz withpicometer displacement resolution. First, we present the study of dynamics of a 2-D micromechanical structure—a MEMSelectrothermal actuator. The structure is realized using SOI MUMPs process from MEMSCAP. The fabricated device is tested for its dynamic performance characteristics using the LDV. In our experiments, we could capture up to 50 out-of-plane modes of vibration—an unprecedented capture—with a single excitation. Subsequent FEM based numerical simulations confirmed that the captured modes were indeed what the experiments indicated, and the measured frequencies werefound to be within 5% of theoretically predicted. Next, we study the dynamics of a 3-D micro droplet and show how the substrate adhesion modulates the natural frequency of the droplet. Adhesion properties of droplets are decided by the degree of wettability that is generally measured by the contact angle between the substrate and the droplet. In this work, we were able to capture 14 modes of vibration of a mercury droplet on different substrates and measure the correspondingfrequencies experimentally. We verify these frequencies with analytical calculations and find that all the measured frequencies are within 6% of theoretically predicted values. We also show that considering any two pairs of natural frequencies, we can calculate the surface tension and the contact angle, thus providing a new method for measuring adhesion of a droplet on an unknown surface. Lastly, we present a study of vibrations of biological cells.Our first study is that of single muscle fibers taken from drosophila.Muscle fibers with different pathological conditions were held in two structural configurations—asa fixed-fixed beam and a cantilever beam—and their vibration signatures analysed.We found that there was significant reduction in natural frequency of diseased fibers. Among the diseased fibers, we could confidently classify the myopathies into nemaline and cardiac types based on the natural frequency of single fibers. We have noticed that the elastic modulus of the muscle which decides the natural frequency is dictated by the myosin expression levels. Our last example isa study of the vibration signatures of cancer cells. Here we measure the natural frequencies of normal and certain cancerous cells, and show that we can distinguish the two based on their natural frequencies. We find that the natural frequency of cancerous cells is approximately half of that of normal cells. Within the cancerous cells, we are able to distinguished epithelial cancer cells and mesenchymal cancer cells based on their natural frequency values. For Epithelial cells,we activate the signaling pathways to induce EMT and notice the reduction in the natural frequency. This mechanical assay based on vibration response corroborates results from the biochemical assays such as Western blots and PCR, thus opening a new technique of mechano-diagnostics.