Phase-separated droplets swim to their dissolution.

Biological macromolecules can condense into liquid domains. In cells, these condensates form membraneless organelles that can organize chemical reactions. However, little is known about the physical consequences of chemical activity in and around condensates. Working with model bovine serum albumin (BSA) condensates, we show that droplets swim along chemical gradients. Active BSA droplets loaded with urease swim toward each other. Passive BSA droplets show diverse responses to externally applied gradients of the enzyme's substrate and products. In all these cases, droplets swim toward solvent conditions that favor their dissolution. We call this behavior "dialytaxis", and expect it to be generic, as conditions which favor dissolution typically reduce interfacial tension, whose gradients are well-known to drive droplet motion through the Marangoni effect. These results could potentially suggest alternative physical mechanisms for active transport in living cells, and may enable the design of fluid micro-robots.

Surface Passivation Method for the Super-repellence of Aqueous Macromolecular Condensates.

Solutions of macromolecules can undergo liquid-liquid phase separation to form droplets with ultralow surface tension. Droplets with such low surface tension wet and spread over common surfaces such as test tubes and microscope slides, complicating in vitro experiments. The development of a universal super-repellent surface for macromolecular droplets has remained elusive because their ultralow surface tension requires low surface energies. Furthermore, the nonwetting of droplets containing proteins poses additional challenges because the surface must remain inert to a wide range of chemistries presented by the various amino acid side chains at the droplet surface. Here, we present a method to coat microscope slides with a thin transparent hydrogel that exhibits complete dewetting (contact angles θ ≈ 180°) and minimal pinning of phase-separated droplets in aqueous solution. The hydrogel is based on a swollen matrix of chemically cross-linked polyethylene glycol diacrylate of molecular weight 12 kDa (PEGDA), and can be prepared with basic chemistry laboratory equipment. The PEGDA hydrogel is a powerful tool for in vitro studies of weak interactions, dynamics, and the internal organization of phase-separated droplets in aqueous solutions.

Soft Deployable Structures via Core-Shell Inflatables.

Deployable structures capable of significant geometric reconfigurations are ubiquitous in nature. While engineering contraptions typically comprise articulated rigid elements, soft structures that experience material growth for deployment mostly remain the handiwork of biology, e.g., when winged insects deploy their wings during metamorphosis. Here we perform experiments and develop formal models to rationalize the previously unexplored physics of soft deployable structures using core-shell inflatables. We first derive a Maxwell construction to model the expansion of a hyperelastic cylindrical core constrained by a rigid shell. Based on these results, we identify a strategy to obtain synchronized deployment in soft networks. We then show that a single actuated element behaves as an elastic beam with a pressure-dependent bending stiffness which allows us to model complex deployed networks and demonstrate the ability to reconfigure their final shape. Finally, we generalize our results to obtain three-dimensional elastic gridshells, demonstrating our approach's applicability to assemble complex structures using core-shell inflatables as building blocks. Our results leverage material and geometric nonlinearities to create a low-energy pathway to growth and reconfiguration for soft deployable structures.

Softness of hydrated salt crystals under deliquescence.

Deliquescence is a first-order phase transition, happening when a salt absorbs water vapor. This has a major impact on the stability of crystalline powders that are important for example in pharmacology, food science and for our environment and climate. Here we show that during deliquescence, the abundant salt sodium sulfate decahydrate, mirabilite (Na2SO4·10H2O), behaves differently than anhydrous salts. Using various microscopy techniques combined with Raman spectroscopy, we show that mirabilite crystals not only lose their facets but also become soft and deformable. As a result, microcrystals of mirabilite simultaneously behave crystalline-like in the core bulk and liquid-like at the surface. Defects at the surface can heal at a speed much faster than the deliquescence rate by the mechanism of visco-capillary flow over the surface. While magnesium sulfate hexahydrate (MgSO4⋅6H2O) behaves similarly during deliquescence, a soft and deformable state is completely absent for the anhydrous salts sodium chloride (NaCl) and sodium sulfate thenardite (Na2SO4). The results highlight the effect of crystalline water, and its mobility in the crystalline structure on the observed softness during deliquescence. Controlled hydrated salts have potential applications such as thermal energy storage, where the key parameter is relative humidity rather than temperature.

Bubble casting soft robotics.

Inspired by living organisms, soft robots are developed from intrinsically compliant materials, enabling continuous motions that mimic animal and vegetal movement1. In soft robots, the canonical hinges and bolts are replaced by elastomers assembled into actuators programmed to change shape following the application of stimuli, for example pneumatic inflation2-5. The morphing information is typically directly embedded within the shape of these actuators, whose assembly is facilitated by recent advances in rapid prototyping techniques6-11. Yet, these manufacturing processes have limitations in scalability, design flexibility and robustness. Here we demonstrate a new all-in-one methodology for the fabrication and the programming of soft machines. Instead of relying on the assembly of individual parts, our approach harnesses interfacial flows in elastomers that progressively cure to robustly produce monolithic pneumatic actuators whose shape can easily be tailored to suit applications ranging from artificial muscles to grippers. We rationalize the fluid mechanics at play in the assembly of our actuators and model their subsequent morphing. We leverage this quantitative knowledge to program these soft machines and produce complex functionalities, for example sequential motion obtained from a monotonic stimulus. We expect that the flexibility, robustness and predictive nature of our methodology will accelerate the proliferation of soft robotics by enabling the assembly of complex actuators, for example long, tortuous or vascular structures, thereby paving the way towards new functionalities stemming from geometric and material nonlinearities.

Drops on the Underside of a Slightly Inclined Wet Substrate Move Too Fast to Grow.

Pendant drops suspended on the underside of a wet substrate are known to accumulate fluid from the surrounding thin liquid film, a process that often results in dripping. The growth of such drops is hastened by their ability to translate over an otherwise uniform horizontal film. Here we show that this scenario is surprisingly reversed when the substrate is slightly tilted (≈2°); drops become too fast to grow and shrink over the course of their motion. Combining experiments and numerical simulations, we rationalize the transition between the conventional growth regime and the previously unknown decay regime we report. Using an analytical treatment of the Landau-Levich meniscus that connects the drop to the film, we quantitatively predict the drop dynamics in the two flow regimes and the value of the critical inclination angle where the transition between them occurs.

Elastic amplification of the Rayleigh-Taylor instability in solidifying melts.

The concomitant mechanical deformation and solidification of melts are relevant to a broad range of phenomena. Examples include the preparation of cotton candy, the atomization of metals, the manufacture of glass fibers, and the formation of elongated structures in volcanic eruptions known as Pele's hair. Usually, solid-like deformations during solidification are neglected as the melt is much more malleable in its initial liquid-like form. Here we demonstrate how elastic deformations in the midst of solidification, i.e., while the melt responds as a very soft solid ([Formula: see text] Pa), can lead to the formation of previously unknown periodic structures. Namely, we generate an array of droplets on a thin layer of liquid elastomer melt coated on the outside of a rotating cylinder through the Rayleigh-Taylor instability. Then, as the melt cures and goes through its gelation point, the rotation speed is increased and the drops stretch into hairs. The ongoing solidification eventually hardens the material, permanently "freezing" these elastic deformations into a patterned solid. Using experiments, simulation, and theory, we demonstrate that the formation of our two-step patterns can be rationalized when combining the tools from fluid mechanics, elasticity, and statistics. Our study therefore provides a framework to analyze multistep pattern formation processes and harness them to assemble complex materials.

Curvature Regularization near Contacts with Stretched Elastic Tubes.

Inserting a rigid object into a soft elastic tube produces conformal contact between the two, resulting in contact lines. The curvature of the tube walls near these contact lines is often large and is typically regularized by the finite bending rigidity of the tube. Here, it is demonstrated using experiments and a Föppl-von Kármán-like theory that a second, independent, mechanism of curvature regularization occurs when the tube is axially stretched. In contrast with the effects of finite bending rigidity, the radius of curvature obtained increases with the applied stretching force and decreases with sheet thickness. The dependence of the curvature on a suitably rescaled stretching force is found to be universal, independent of the shape of the intruder, and results from an interplay between the longitudinal stresses due to the applied stretch and hoop stresses characteristic of curved geometry. These results suggest that curvature measurements can be used to infer the mechanical properties of stretched tubular structures.

Stains from Freeze-Dried Drops.

The evaporation of droplets of colloidal suspensions onto a surface is a common tool to achieve surface coatings and self-assembly. However, because of the spontaneous flow developing within an evaporating drop, the deposit is difficult to control, and an unwanted ring-like structure often forms, with particles aggregating along the drop edge. Here, by freezing the drops before sublimating them in dry air we propose a new approach that produces a different kind of stain where most particles are clustered in the center of the drops instead. We demonstrate that these deposits can be continuously tuned from wide but thin to concentrated and thick by varying the droplet's aspect ratio. Unlike evaporated liquid drops, stains from freeze-dried drops do not depend on the drying conditions or substrate roughness and possess a porous and branched microstructure somewhat reminiscent of freeze-casted ceramics. With these stains being governed by the freezing process rather than the drying, this opens alternative ways to control colloidal deposits.

Singular sublimation of ice and snow crystals.

The evaporation (sublimation) of ice and snow has a major impact on global climate, since the amount of ice and snow determines Earth's albedo. Yet, due to their complex geometry with several sharp regions which are singular for the evaporation, the precise evaporation dynamics of snow and ice crystals remains challenging to predict. Here, we study the sublimation of snowflakes and pointy ice drops. We show that the evaporation rates of water and ice drops are similar; they are both limited by the diffusive transport of the vapour. This allows us to predict ice and snowflake evaporation quantitatively by solving the diffusive free-boundary problem, which correctly predicts the rapid self-similar evolution of sharp edges and points. Beyond providing a conceptual picture to understand the sublimation of ice crystals, our results are more generally applicable to other diffusion problems such as the dissolution of salt crystals or pharmaceuticals.

Drops Floating on Granular Rafts: A Tool for Liquid Transport and Delivery.

Solid particles can modify the properties of liquid interfaces and are therefore widely used to coat drops, bubbles, and stabilize emulsions and foams. Here, we propose a new, easy, and affordable method to produce millimetric to centimetric water-in-water capsules using solid particles. We prevent the coalescence of a water drop at an oil-water interface using a monolayer of large, dense, and hydrophobic particles: a "granular raft". The capsule is then formed by a mechanical instability occurring when the interface collapses under the combined load of the floating drop and particle weight. During the destabilization, the water drop sinks into the water subphase through an oil-particle film which covers it to produce the armored capsule. By modeling the raft as a heavy membrane, we predict the floating drop shape, the raft deformation, its destabilization and highlight the complex dual nature (solid- and liquid-like) of the capsule shell. Because armored capsules' content is isolated, transportable, and easily releasable, they are great candidates for applications requiring transport of water-soluble compounds in aqueous systems such as green chemistry or cell biology.

The compression of a heavy floating elastic film.

We study the effect of film density on the uniaxial compression of thin elastic films at a liquid-fluid interface. Using a combination of experiments and theory, we show that dense films first wrinkle and then fold as the compression is increased, similarly to what has been reported when the film density is neglected. However, we highlight the changes in the shape of the fold induced by the film's own weight and extend the model of Diamant and Witten [Phys. Rev. Lett., 2011, 107, 164302] to understand these changes. In particular, we suggest that it is the weight of the film that breaks the up-down symmetry apparent from previous models, but elusive experimentally. We then compress the film beyond the point of self-contact and observe a new behaviour dependent on the film density: the single fold that forms after wrinkling transitions into a closed loop after self-contact, encapsulating a cylindrical droplet of the upper fluid. The encapsulated drop either causes the loop to bend upward or to sink deeper as the compression is increased, depending on the relative buoyancy of the drop-film combination. We propose a model to qualitatively explain this behaviour. Finally, we discuss the relevance of the different buckling modes predicted in previous theoretical studies and highlight the important role of surface tension in the shape of the fold that is observed from the side-an aspect that is usually neglected in theoretical analyses.

Self-consistent field theory for the interactions between keratin intermediate filaments.

BACKGROUND: Keratins are important structural proteins found in skin, hair and nails. Keratin Intermediate Filaments are major components of corneocytes, nonviable horny cells of the Stratum Corneum, the outermost layer of skin. It is considered that interactions between unstructured domains of Keratin Intermediate Filaments are the key factor in maintaining the elasticity of the skin. RESULTS: We have developed a model for the interactions between keratin intermediate filaments based on self-consistent field theory. The intermediate filaments are represented by charged surfaces, and the disordered terminal domains of the keratins are represented by charged heteropolymers grafted to these surfaces. We estimate the system is close to a charge compensation point where the heteropolymer grafting density is matched to the surface charge density. Using a protein model with amino acid resolution for the terminal domains, we find that the terminal chains can mediate a weak attraction between the keratin surfaces. The origin of the attraction is a combination of bridging and electrostatics. The attraction disappears when the system moves away from the charge compensation point, or when excess small ions and/or NMF-representing free amino acids are added. CONCLUSIONS: These results are in concordance with experimental observations, and support the idea that the interaction between keratin filaments, and ultimately in part the elastic properties of the keratin-containing tissue, is controlled by a combination of the physico-chemical properties of the disordered terminal domains and the composition of the medium in the inter-filament region.