Drop impact dynamics of complex fluids: a review.

The impact of fluid drops on solid substrates has widespread interest in many industrial coating and spraying applications, such as ink-jet printing and agricultural pesticide sprays. Many of the fluids used in these applications are non-Newtonian, that is they contain particulate or polymeric additives that strongly modify their flow behaviour. While a large body of experimental and theoretical work has been done to understand the impact dynamics of Newtonian fluids, we as a community have much progress to make to understand how these dynamics are modified when the impact fluid has non-Newtonian rheology. In this review, we outline recent experimental, theoretical, and computational advances in the study of impact dynamics of complex fluids on solid surfaces. Here, we provide an overview of this field that is geared towards a multidisciplinary audience. Our discussion is segmented by two principal material constitutions: polymeric fluids and particulate suspensions. Throughout, we highlight promising future directions, as well as ongoing experimental and theoretical challenges in the field.

A simple catch: Fluctuations enable hydrodynamic trapping of microrollers by obstacles.

It is known that obstacles can hydrodynamically trap bacteria and synthetic microswimmers in orbits, where the trapping time heavily depends on the swimmer flow field and noise is needed to escape the trap. Here, we use experiments and simulations to investigate the trapping of microrollers by obstacles. Microrollers are rotating particles close to a bottom surface, which have a prescribed propulsion direction imposed by an external rotating magnetic field. The flow field that drives their motion is quite different from previously studied swimmers. We found that the trapping time can be controlled by modifying the obstacle size or the colloid-obstacle repulsive potential. We detail the mechanisms of the trapping and find two remarkable features: The microroller is confined in the wake of the obstacle, and it can only enter the trap with Brownian motion. While noise is usually needed to escape traps in dynamical systems, here, we show that it is the only means to reach the hydrodynamic attractor.

Heterogeneity-stabilized homogeneous states in driven media.

Understanding the relationship between symmetry breaking, system properties, and instabilities has been a problem of longstanding scientific interest. Symmetry-breaking instabilities underlie the formation of important patterns in driven systems, but there are many instances in which such instabilities are undesirable. Using parametric resonance as a model process, here we show that a range of states that would be destabilized by symmetry-breaking instabilities can be preserved and stabilized by the introduction of suitable system asymmetry. Because symmetric states are spatially homogeneous and asymmetric systems are spatially heterogeneous, we refer to this effect as heterogeneity-stabilized homogeneity. We illustrate this effect theoretically using driven pendulum array models and demonstrate it experimentally using Faraday wave instabilities. Our results have potential implications for the mitigation of instabilities in engineered systems and the emergence of homogeneous states in natural systems with inherent heterogeneities.

Gel rupture during dynamic swelling.

Hydrogels have had a profound impact in the fields of tissue engineering, drug delivery, and materials science as a whole. Due to the network architecture of these materials, imbibement with water often results in uniform swelling and isotropic expansion which scales with the degree of cross-linking. However, the development of internal stresses during swelling can have dramatic consequences, leading to surface instabilities as well as rupture or bursting events. To better understand hydrogel behavior, macroscopic mechanical characterization techniques (e.g. tensile testing, rheometry) are often used, however most commonly these techniques are employed on samples that are in two distinct states: (1) unswollen and without any solvent, or (2) in an equilibrium swelling state where the maximum amount of water has been imbibed. Rarely is the dynamic process of swelling studied, especially in samples where rupture or failure events are observed. To address this gap, here we focus on rupture events in poly(ethylene glycol)-based networks that occur in response to swelling with water. Rupture events were visualized using high-speed imaging, and the influence of swelling on material properties was characterized using dynamic mechanical analysis. We find that rupture events follow a three-stage process that includes a waiting period, a slow fracture period, and a final stage in which a rapid increase in the velocity of crack propagation is observed. We describe this fracture behavior based on changes in material properties that occur during swelling, and highlight how this rupture behavior can be controlled by straight-forward modifications to the hydrogel network structure.

Driven dynamics in dense suspensions of microrollers.

We perform detailed computational and experimental measurements of the driven dynamics of a dense, uniform suspension of sedimented microrollers driven by a magnetic field rotating around an axis parallel to the floor. We develop a lubrication-corrected Brownian dynamics method for dense suspensions of driven colloids sedimented above a bottom wall. The numerical method adds lubrication friction between nearby pairs of particles, as well as particles and the bottom wall, to a minimally-resolved model of the far-field hydrodynamic interactions. Our experiments combine fluorescent labeling with particle tracking to trace the trajectories of individual particles in a dense suspension, and to measure their propulsion velocities. Previous computational studies [B. Sprinkle et al., J. Chem. Phys., 2017, 147, 244103] predicted that at sufficiently high densities a uniform suspension of microrollers separates into two layers, a slow monolayer right above the wall, and a fast layer on top of the bottom layer. Here we verify this prediction, showing good quantitative agreement between the bimodal distribution of particle velocities predicted by the lubrication-corrected Brownian dynamics and those measured in the experiments. The computational method accurately predicts the rate at which particles are observed to switch between the slow and fast layers in the experiments. We also use our numerical method to demonstrate the important role that pairwise lubrication plays in motility-induced phase separation in dense monolayers of colloidal microrollers, as recently suggested for suspensions of Quincke rollers [D. Geyer et al., Phys. Rev. X, 2019, 9(3), 031043].

Magneto-capillary dynamics of amphiphilic Janus particles at curved liquid interfaces.

A homogeneous magnetic field can exert no net force on a colloidal particle. However, by coupling the particle's orientation to its position on a curved interface, even static homogeneous fields can be used to drive rapid particle motions. Here, we demonstrate this effect using magnetic Janus particles with amphiphilic surface chemistry adsorbed at the spherical interface of a water drop in decane. Application of a static homogeneous field drives particle motion to the drop equator where the particle's magnetic moment can align parallel to the field. As explained quantitatively by a simple model, the effective magnetic force on the particle scales linearly with the curvature of the interface. For particles adsorbed on small droplets such as those found in emulsions, these magneto-capillary forces can far exceed those due to magnetic field gradients in both magnitude and range. This mechanism may be useful in creating highly responsive emulsions and foams stabilized by magnetic particles.

The role of rigidity in controlling material failure.

We investigate how material rigidity acts as a key control parameter for the failure of solids under stress. In both experiments and simulations, we demonstrate that material failure can be continuously tuned by varying the underlying rigidity of the material while holding the amount of disorder constant. As the rigidity transition is approached, failure due to the application of uniaxial stress evolves from brittle cracking to system-spanning diffuse breaking. This evolution in failure behavior can be parameterized by the width of the crack. As a system becomes more and more floppy, this crack width increases until it saturates at the system size. Thus, the spatial extent of the failure zone can be used as a direct probe for material rigidity.

Geometric control of failure behavior in perforated sheets.

Adding perforations to a continuum sheet allows new modes of deformation, and thus modifies its elastic behavior. The failure behavior of such a perforated sheet is explored, using a model experimental system: a material containing a one-dimensional array of rectangular holes. In this model system, a transition in failure mode occurs as the spacing and aspect ratio of the holes are varied: rapid failure via a running crack is completely replaced by quasistatic failure, which proceeds via the breaking of struts at random positions in the array of holes. I demonstrate that this transition can be connected to the loss of stress enhancement, which occurs as the material geometry is modified.

Creation of prompt and thin-sheet splashing by varying surface roughness or increasing air pressure.

A liquid drop impacting a solid surface may splash either by emitting a thin liquid sheet that subsequently breaks apart or by promptly ejecting droplets from the advancing liquid-solid contact line. Using high-speed imaging, we show that surface roughness and air pressure influence both mechanisms. Roughness inhibits thin-sheet formation even though it also increases prompt splashing at the advancing contact line. If the air pressure is lowered, droplet ejection is suppressed not only during thin-sheet formation but also for prompt splashing.

Ultrafast interference imaging of air in splashing dynamics.

A drop impacting a solid surface with sufficient velocity will emit many small droplets creating a splash. However, splashing is completely suppressed if the surrounding gas pressure is lowered. The mechanism by which the gas affects splashing remains unknown. We use high-speed interference imaging to measure the air beneath all regions of a spreading viscous drop as well as optical absorption to measure the drop thickness. Although an initial air bubble is created on impact, no significant air layer persists until the time a splash is created. This suggests that splashing in our experimentally accessible range of viscosities is initiated at the edge of the drop as it encroaches into the surrounding gas.

Thin film formation during splashing of viscous liquids.

After impact onto a smooth dry surface, a drop of viscous liquid initially spreads in the form of a thick lamella. If the drop splashes, it first emits a thin fluid sheet that can ultimately break up into droplets causing the splash. Ambient gas is crucial for creating this thin sheet. The time for sheet ejection, t{ejt}, depends on impact velocity, liquid viscosity, gas pressure, and molecular weight. A central air bubble is trapped below the drop at pressures even below that necessary for this sheet formation. In addition, air bubbles are entrained underneath the spreading lamella when the ejected sheet is present. Air entrainment ceases at a lamella velocity that is independent of drop impact velocity as well as ambient gas pressure.