Pattern formation, i.e., the outcome of self-organization, has fascinated scientists for centuries. A large effort was devoted to understand the formation of regular patterns in dissipative structures. More recently, it appears that self-organized structures could also be achieved near equilibrium. There is a great variety of physical and chemical systems that, near equilibrium, exhibit periodic patterns. For instance, stripes or bubbles could be observed in thin films of magnetic garnet, superconducting materials, block copolymers, liquid crystals, phospholipids, and ferrofluids. Wrinkling instability of compressed rigid membranes on soft elastic substrates leads also to the formation of periodic patterns near equilibrium. Since the seminal paper of Bowden et al. (Nature 1998), various systems were proposed to generate nano- and micrometric wrinkles via the application of compressive stresses to multilayers. In addition to its purely fundamental interest, these instabilities also offer a new route to build in a simple, cost-effective, and well-defined way nano- and microstructured surfaces without the use of the traditional, robust techniques developed in the microelectronics industry. In this thesis, we develop a new system, metal-polymer-substrate trilayers, that exhibit wrinkling when heated above the glass transition temperature of the polymer. We explain in detail the mechanism at the origin of wrinkling and expand existing models to obtain a complete description of the relevant parameters that govern both the amplitude and the wavelength of the obtained pattern. In light of this, we show that by playing with the rheological properties of the polymer we are able to control precisely the geometry of the wrinkles. Furthermore, to generate surfaces with a tailor-made buckling pattern, we develop an original variant of the experiments. We tune the boundary conditions at the polymer-substrate interface by chemically patterning the substrates with regions of high and low adhesion. In this way, we obtain patterns with wrinkles being oriented differently above the sticky and the slippery regions. This last result is very surprising since it seems, at first sight, unrealistic to imagine that the chemical nature of the substrate could affect the elastic instability of the skin through a micron-thick polymer film. To explore wrinkled patterns with complex morphologies, we couple the wrinkling instability with solvent diffusion. Molecular diffusion in the polymer layer triggers the transition from an unwrinkled to a wrinkled state, provided that stimuloresponsive mutlilayers are used. The wrinkled pattern obtained is determined by the geometry of the diffusion process. To understand this surprising observation, we explain in detail how the scalar field related to the solvent concentration affects so strongly the elastic instabilities usually determined by the tensorial stress field. This mechanism allows us thus to grant exotic stress distributions which lead to very intriguing patterns (e.g. parallel or radial folds, herringbones). Interestingly, we find that under specific conditions, a hierarchical wrinkled morphology, i.e. pattern of wrinkles branching into generations of ever-higher folds, develops. We study other manifestations of hierarchical structures existing around us. In this frame, we derive a general concept that a plate constrained at one edge (with a fixed wavelength) but free at the opposite one evolves naturally to larger wavelengths to minimize its bending energy. We show theoretically that the evolution results from a compromise between the gain in bending energy and the energetic penalties related to the change of wavelength. We demonstrate the universality of these concepts by showing that our commonplace suspended curtain behaves like nanometer-thick polystyrene films deposited on water and further compressed. We close this thesis by making a short review of the main applications related to wrinkling that are already described in literature and develop in detail one of them, the use of wrinkling to investigate cell contact guidance.

In the study, we confer with the effect of the circular cylinder for various flow fields, and investigate the phenomenon of the vortex shedding and fluid elastic instabilities. First, in the aspect of the vortex shedding, we observe the wake behind the cylinder after varying the locations of orifices on the cylinder and the forms of momentum addition, and the variation of the lift and drag coefficient can be obtained by using the commercial software STAR-CD. In the further study, we make the type of flow field to be a shear flow and build the database of the aerodynamic coefficients in different shear parameter and Reynolds numbers; furthermore, the database is an important basis for us to conjecture the surface force on the cylinder, and analyze the size of oscillations and the orbit that is caused by the shear parameter, mass ratio and damping factor respectively.

Slender structures like plates and shells -- for which at least one dimension is much smaller than the others -- are lightweight, flexible, and offer considerable strength with little material. As such, these structures are abundant in nature (e.g. flower petals, eggshells, and blood vessels) and design (e.g. bridge decks, fuel tanks, and soda cans). However, with slenderness comes suceptibility to large and often sudden deformations, which can be wildly nonlinear, as bending is energetically preferable to stretching. Though once considered categorically undesirable, these instabilities are often coveted nowadays in the engineering community. They provide mechanical explanations for observations in nature like the wrinkled structure of the brain or the snapping mechanism of the Venus fly trap, and when precisely controlled, enable the design of functional devices like artificial muscles or self-propelling microswimmers. As a prerequisite, these achievements require a thorough understanding of how thin structures "shape-shift" in response to stimuli and confinement. Advancing this fundamental knowledge is the goal of this thesis. In the first two chapters, we consider the shape-selection of shells and plates that are confined by their environment. The shells are made by residual swelling of silicone elastomers, a process that mimics differential growth, and causes initially flat structures to irreversibly morph into curved shapes. Flattening the central region forces further reconfiguration, and the confined shells display multi-lobed buckling patterns. These experiments, finite element (FE) simulations, and a scaling argument reveal that a single geometric confinement parameter predicts the general features of this shape-selection. Next, in experiments and molecular dynamics (MD) simulations, we constrain intrinsically flat sheets in the same manner, so that their center remains flat when we quasi-statically force them through a ring. In the absence of planar confinement, these sheets form a well-studied conical shape (the developable cone or d-cone). Our annular d-cone buckles circumferentially into patterns that are qualitatively similar to the confined shells, despite the distinct curvatures and loading methods. This is explained by the dominant role of confinement geometry in directing deformation, which we uncover via a scaling argument based on the elastic energy. There are also marked differences between the way plates and shells change shape, which we highlight when we investigate the rich dynamics of reconfiguration. In the final two chapters, we demonstrate how mechanics, geometry, and materials can inform the design of structures that use instabilities to function. We observe in experiments that dynamic loading causes a spherical elastomer shell to buckle at ostensibly subcritical pressures, following a substantial time delay. To explain this, we show that viscoelastic creep deformation lowers the critical load in the same predictable, quantifiable way that a growing defect would in an elastic shell. This work offers a pathway to introduce tunable, time-controlled actuation to existing mechanical actuators, e.g. pneumatic grippers. The final chapter aims at reducing the energy input required for bistable actuators, wherein snap-through instability is typically induced by a stimulus applied to the entire shell. To do so, we combine theory with 1D finite element simulations of spherical caps with a non-homogeneous distribution of stimuli--responsive material. We demonstrate that restricting the active area to the shell boundary allows for a large reduction in its size, while preserving snap-through behavior. These results are stimulus-agnostic, which we demonstrate with two sets of experiments, using residual swelling of bilayer silicone elastomers as well as a magneto-active elastomer. Our findings elucidate the underlying mechanics, offering an intuitive route to optimal design for efficient snap-through. / 2022-05-06T00:00:00Z

L’écoulement et la stabilité des rideaux liquides viscoélastiques sont étudiés pour des solutions de polymères flexibles et semi rigides. Ces liquides viscoélastiques sont extrudés à partir d’une fente à débit constant et s’écoulent à l’air libre sous l’effet de la gravité. L’écoulement de ces liquides se caractérise par un équilibre initial entre la gravité et les forces élastiques causées par les déformations des chaînes de polymère, jusqu’à ce que l’inertie du liquide finisse par dominer et que l’on retrouve le comportement classique de chute libre. Nous montrons que l’écoulement est principalement influencé par la valeur du temps de relaxation extensionnel mesuré par une méthode de filamentation. Un nouvel éclairage sur l’écoulement des rideaux liquides Newtoniens nous permet de trouver une courbe maîtresse de l’écoulement dans le cas viscoélastique par analogie. En ce qui concerne la stabilité du rideau, nous observons que le débit critique de formation du rideau n’est pas affecté par la présence de polymères, tandis que le débit minimum en deçà duquel le rideau se rompt diminue après ajout de polymères, ce qui révèle une plus grande résistance de la nappe à l’initiation de trous. Par ailleurs, nous observons une instabilité de l’écoulement pour les solutions les plus rhéofluidifiantes, où des bandes épaisses (où la vitesse du liquide est supérieure à la moyenne) sont formées au sein du rideau. Une visualisation de l’écoulement à l’intérieur de la filière d’extrusion révèle que ce phénomène est lié à une instabilité de l’écoulement de contraction en amont de la fente, où l’écoulement est de nature instationnaire et tridimensionnelle. / The flow and the stability of viscoelastic liquid curtains are investigated using solutions of flexible and semi-rigid polymer chains. These viscoelastic liquids are extruded from a slot at constant flow rate and fall in ambient air under gravity. We show that the curtain flow of polymer solutions is characterized by an initial balance between gravity and the elastic stresses arising from the stretching of polymer molecules, until inertia finally dominates and the classical free-fall behavior is recovered. We show that the flow is mostly influenced by the value of the extensional relaxation time of the solution measured by a filament thinning technique. New insights on the theoretical description of Newtonian curtains allow us to find the master curve of the viscoelastic curtain flow by analogy. Concerning the curtain stability, we show that the critical flow rate for curtain formation is not affected by the presence of polymers whereas the minimum flow rate below which the curtain rapidly breaks is reduced by polymer addition, thus revealing a greater resistance of the sheet to hole initiations. Furthermore, we observe the onset of a flow instability for the most shear-thinning solutions, where thick bands (where the liquid velocity is larger than average) are formed within the curtain. Visualizations of the flow inside the die reveal that this phenomenon is linked to a flow instability at the contraction plane upstream of the slot where the flow is unsteady and three-dimensional in nature

Dans cette thèse à l’interface entre élasticité et capillarité, nous présentons tout d’abord une instabilité élastique, le claquage, revisitée dans un contexte élastocapillaire. En déposant une goutte d’eau sous une lamelle flambée en position basse, nous parvenons à déclencher une instabilité de claquage à contresens de la gravité. Cette démonstration de la prédominance des effets capillaires à petite échelle s’accompagne d’une étude des positions d’équilibre et de la stabilité de systèmes goutte-lamelle. Nous démontrons l’influence importante de la taille et de la position de la goutte le long de la lamelle, puis étendons notre étude au cas de bulles ou de gouttes condensées à partir de vapeur d’eau. Enfin, nous nous intéressons à l’aspect dynamique de l’instabilité, qui est dictée principalement par l’élasticité, y compris dans le cas élastocapillaire.Nous mettons ensuite en évidence un phénomène surprenant : la dynamique de descente d’une goutte d’eau sur un élastomère silicone présente deux régimes successifs, caractérisés par deux vitesses différentes. Nous montrons que les chaînes libres non réticulées présentes dans l’élastomère sont à l’origine de cette dynamique inattendue. La goutte est progressivement recouverte par des chaînes de silicone, et sa vitesse change brutalement lorsqu’une concentration surfacique critique est atteinte, ce qui se traduit par une transition brutale de tension de surface. Nous nous intéressons aux vitesses de gouttes dans les deux régimes ainsi qu’aux échelles de temps mises en jeu lors de l’extraction de chaînes non réticulées, et montrons que l’extraction de ces chaînes se produit au niveau de la ligne triple. / This thesis focuses on interactions between liquids and elastic solids. We first revisit the snap-through instability from an elastocapillary point of view, showing that capillary forces are able to counterbalance gravity by inducing snap-through with a droplet deposited below a downward buckled elastic strip clamped at both ends. Equilibrium, stability, and dynamics of drop-strip systems are investigated, demonstrating the influence of droplet size and droplet position along the buckled strip, and showing that capillarity is driving the system toward instability but elasticity is ruling the subsequent dynamics. Spin-off versions of the experiment are also designed, including a humidity-controlled mechanical switch and upscaled experiments using soap bubbles.We then focus on interactions between silicone elastomers and aqueous droplets to understand the mechanisms underlying an unexpected two-regime droplet dynamics observed on vertical silicone elastomer plates. After demonstrating that this two-regime dynamics is due to the presence of uncrosslinked oligomers in the elastomer, we show that the speed transition coincides with a surface tension transition. A quantitative study of the droplets speeds in the two regimes is performed, and the timescale needed for uncrosslinked oligomers to cover the water-air interface is investigated both for sessile and moving droplets. We eventually show that uncrosslinked chains are extracted from the elastomer at the water - air - silicone elastomer triple line, and demonstrate that extraction occurs in various setups such as partially immersed silicone elastomer plates or air bubbles sliding up PDMS planes immersed in a water bath.

In day to day life we encounter many different materials which are intermediate between crystalline solids and simple liquids that include paints , glues , suspensions, polymers, surfactants, food and cosmetic products and so on. ‘Soft condensed matter’ is an emerging field of science that aims to generalize the flow and various deformation mechanisms in this apparent diverse class of materials from a ‘mesoscopic’ point of view (important length scales for these systems is usually 10nm-1μm) where the actual atomic and molecular details governed by various quantum mechanical laws are not very important. These soft systems are held together by weaken tropic forces and therefore can be perturbed easily (the typical elastic modulus of these materials is many orders of magnitude lower compared to metallic solids). Moreover, very long relaxation times in these systems(∼10−3 to 1 s) have made them ideal candidates to study non-equilibrium physics. The present Thesis is an endeavor to understand linear and non-linear flow behavior and low Reynolds number instabilities in various soft matter systems like suspensions of flocculated carbon nanotubes and carbon black, surfactant gels, colloidal glasses, Langmuir monolayers etc probed mainly by bulk and interfacial rheology, in-situ light scattering, particle image velocimetry(PIV) techniques and Fourier transform rheology. We also use dynamic light scattering techniques for particle sizing and characterization of Brownian systems. Chapter 1 gives a general introduction to soft condensed matter, particularly, the important length and time scales, various interactions and the rich phase behavior emerged from the delicate balance between energy and entropy in these systems. In this context, We describe the detailed phase behavior of two such systems studied in this thesis. We next describe briefly a few important concepts which motivate the main problems studied in the present thesis like the shear-thickening in suspensions of Brownian and non-Brownian particles, non-equilibrium steady state fluctuation relations in driven systems, elasticity driven instabilities in complex fluids, jamming transitions and aging behavior. This is followed by a discussion of the experimental techniques like linear and nonlinear rheology, including the Fourier transform rheology. Chapter 2 discusses the experimental techniques used by us in detail. We first describe the different components and mode of operations of the MCR-300 stress-controlled rheometer (Paar Physica, Germany) and various experimental geometries. Next we discuss the set up for two dimensional rheological measurements. The homebuilt imaging set up for in-situ polarized light scattering and direct imaging studies is described along with the in-situ particle image velocimetry (PIV) to map out the exact spatially resolved velocity profiles in 2D systems. We give a brief account of the techniques of Fourier transform rheology. At the end of this chapter, we briefly describe the angle resolved dynamic light scattering (DLS) set up (Brookhaven Instruments, USA). In Chapter 3, we study colossal discontinuous shear-thickening transition in confined suspensions of fractal clusters formed by multi-wall carbon nanotubes (MWNT) by rheology and in-situ imaging experiments. Monotonic decrease in viscosity with increasing shear stress, known as shear thinning, is a known rheological response to shear flow in complex fluids in general and for flocculated suspensions in particular. In the present experiments we demonstrate a discontinuous shear thickening transition where the viscosity jumps sharply above a critical shear stress by four to six orders of magnitude in flocculated suspensions of MWNT even at very low weight fractions(∼0.5%). Rheo-optical observations reveal the shear-thickened state as a percolated structure of MWNT flocs spanning the system size. We present a dynamic phase diagram of the non-Brownian MWNT dispersions revealing a starting jammed state followed by shear-thinning and shear-thickened states. The present study further suggests that the shear-thickened state obtained as a function of shear stress is likely to be a generic feature of fractal clusters under flow, albeit under confinement. An understanding of the shear thickening phenomena in confined geometries is pertinent for flow controlled fabrication techniques in enhancing the mechanical strength and transport properties of thin films and wires of nanostructured composites as well as in lubrication issues. We try to understand the flow of jammed and shear-thickened states under constant applied strain rate by studying the building up and relaxation of individual stress fluctuation events similar to the flow in dense granular materials. We also characterize the metastable shear thickened states by superposing a small sinusoidal stress component on a steady applied stress as well as by studying the a thermal entropy consuming fluctuations which are also observed for other jammed systems under an applied steady shear stress as described in the next chapter. Chapter 4 reports the study of non-equilibrium fluctuations in concentrated gels and glassy systems(in jammed state), the nature of fluctuations and their systemsize dependence in the framework of fluctuation relation and Generalized Gumbel distribution. In the first part, we show that the shear rate at a fixed shear stress in a micellar gel in a jammed state exhibits large fluctuations, showing positive and negative values, with the mean shear rate being positive. The resulting probability distribution functions (PDFs) of the global power flux to the system vary from Gaussian to non-Gaussian, depending on the driving stress and in all cases show similar symmetry properties as predicted by Gallavotti-Cohen steady state fluctuation relation. The fluctuation relation allows us to determine an effective temperature related to the structural constraints of the jammed state. We have measured the stress dependence of the effective temperature. Further, experiments reveal that the effective temperature and the standard deviation of the shear rate fluctuations increase with the decrease of the systemsize. In the second part of this chapter, we report a universal large deviation behavior of spatially averaged global injected power just before the rejuvenation of the jammed state formed by an aging suspension of laponite clay under an applied stress. The probability distribution function (PDF) of these entropy consuming strongly non-Gaussian fluctuations follow an universal large deviation functional form described by the Generalized Gumbel (GG) distribution like many other equilibrium and non-equilibrium systems with high degree of correlations but do not obey Gallavotti-Cohen Steady State Fluctuation Relation (SSFR). However, far from the unjamming transition (for smaller applied stresses) SSFR is satisfied for both Gaussian as well as non-Gaussian PDF. The observed slow variation of the mean shear rate with system size supports a recent theoretical prediction for observing GG distribution. We also establish the universality of the observations reported in this chapter in the light of other jammed systems under shear. We examine in the first part of Chapter 5, the shear-thinning behavior of a two dimensional yield stress bearing monolayer of sorbitan tristearate at air/water interface. The flow curve (stress vs shear rate) consists of a linear region at low shear stresses/shear rates, followed by a stress plateau at higher values. The velocity profile obtained from particle imaging velocimetry indicates that shear banding occurs showing coexistence of fluidized region near the rotor and solid region with vanishing shear-rate away from the rotor. In the fluidized region, the velocity profile which is linear at low shear rates becomes exponential at the onset of shear-thinning, followed by a time varying velocity profile in the plateau region. At low values of constant applied shear rates, the viscosity of the film increases with time, thus showing aging behavior like in soft glassy three-dimensional (3D) systems. Further, at the low values of the applied stress in the yield stress regime, the shear-rate fluctuations in time show both positive and negative values, similar to that observed in sheared 3D jammed systems. By carrying out a statistical analysis of these shear-rate fluctuations, we estimate the effective temperature of the soft glassy monolayer using the Galavatti-Cohen steady state fluctuation relation. In the second part of this chapter, we study in detail the non-linear viscoelastic behavior of Langmuir monolayers. Under oscillatory shear usually observed in many 3D metastable complex fluids with large structural relaxation times. At large strain amplitudes(γ), the storage modulus (G”) decreases monotonically whereas the loss modulus (G”) exhibits a peak above a critical strain amplitude before it decreases at higher strain amplitudes. The power law decay exponents of G” and G” are in the ratio 2:1. The peak in G” is absent at high temperatures and low concentration of sorbitan tristearate. Strain-rate frequency sweep measurements on the monolayers do indicate a strain-rate dependence of the structural relaxation time. The present study on sorbitan tristearate monolayers clearly indicates that the nonlinear viscoelastic behavior in 2D Langmuir monolayers is very general and exhibits many of the features observed in 3D complex fluids. We report in the first part of Chapter 6 scattering dichroism experiments to quantify the spatio-temporal nematodynamics of shear-thinning worm like micellar gels of surfactant Cetyltrimethylammonium Tosylate (CTAT) in the presence of salt sodium chloride (NaCl) enroute to rheochaos. For shear rates past the plateau onset, we observe a presence of alternating bright and dark‘ intertwined’ birefringent structures along the vorticity direction. The orientational order corresponding to these structures are predominantly oriented at +45deg and−45deg to the flow (v) in the (v,∇v) plane. The orientational dynamics of the nematics especially at the interface between the structures, has a one-to-one correspondence with the temporal behavior of the stress. Experiments show that the spatial motion of the vorticity structures depend on the gap thickness of the Couette cell. We next discuss the random temporal flow behavior of this system at high values of applied shear rate/stress in the framework of elastic turbulence in the second part of this chapter. Here, we study the statistical properties of spatially averaged global injected power fluctuations for the worm-like micellar system described above. At sufficiently high Weissenberg numbers (Wi) the shear rate and hence the injected power p(t) at a constant applied stress shows large irregular fluctuations in time. The nature of the probability distribution function (PDF) of p(t) and the power-law decay of its power spectrum are very similar to that observed in recent studies of elastic turbulence for polymer solutions. Remarkably, these non-Gaussian pdf scan be well described by an universal large deviation functional form given by the Generalized Gumbel (GG) distribution observed in the context of spatially averaged global measures in diverse classes of highly correlated systems. We show by in-situ rheology and polarized light scattering experiments that in the elastic turbulent regime the flow is spatially smooth but random in time, in agreement with a recent hypothesis for elastic turbulence. In Chapter 7, we study the vorticity banding under large amplitude oscillatory shear (LAOS) in a dilute worm-like micellar gel formed by surfactant CTAT by Fourier transform rheology and in-situ polarized light scattering. Under LAOS we found the signature of a non-trivial order-disorder transition of Taylor vortices. In the non-linear regime, higher harmonicde composition of the resulting stress signal reveals that the third harmonic I3 shows a very prominent maximum at the strain value where the number density (nv) of the Taylor vortices is maximum for a wide range of angular frequencies both above and below the linear crossover point. Subsequent increase in applied strain results in distortions of the vortices and a concomitant decrease in nv when I3 also drops very sharply and acts like an order parameter for this order-disorder transition. We further quantify the transition by defining an independent order parameter like quantity from the spatial correlation function of the scattered intensity and equivalently its Fourier transform which essentially captures the non monotonous third harmonic behavior. Lissajous plots indicate an intra-cycle strain hardening for the values of γ corresponding to the peak of I3 similar to that observed for hard-sphere glasses. Our study is an important step forward to correlating the structures developed in the system under LAOS to the appearances of the higher harmonics in the non-linear regime. The Thesis concludes with a summary of the main results and a brief account on the scope of future work as described in Chapter 8.