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Robert W. Style

Publications and source records attributed to Robert W. Style.

At least 37 records · Page 2Linked to original sources

Stress accumulation around ice in a temperature gradient

When materials freeze, they often undergo damage due to ice growth. Although this damage is commonly ascribed to the volumetric expansion of water upon freezing, it is usually driven by suction of water towards growing ice crystals. The freezing of this additional water can cause a large build up of stress. Here, we study this process by producing a stable ice/water interface in a controlled temperature gradient, and measuring the deformation of the confining boundary. Analysis of the deformation field reveals stresses applied to the boundary with $\mathcal{O}(μ\mathrm{m})$ resolution. Globally, stresses increase steadily over time as liquid water is transported to more deeply undercooled regions. Locally, stresses increase until ice growth is stalled by the confining stresses. In accordance with the Clapeyron equation, the local limiting stress is proportional to the local undercooling. These results are closely connected to the crystallization pressure for growing crystals and condensation pressure during liquid-liquid phase separation.

cond-mat.soft↗

Dynamics of Spontaneous Wrapping of Microparticles by Floppy Lipid Membranes

Lipid membranes form the barrier between the inside and outside of cells and many of their subcompartments. As such, they bind to a wide variety of nano- and micrometer sized objects and, in the presence of strong adhesive forces, strongly deform and envelop particles. This wrapping plays a key role in many healthy and disease-related processes. So far, little work has focused on the dynamics of the wrapping process. Here, using a model system of micron-sized colloidal particles and giant unilamellar lipid vesicles with tunable adhesive forces, we measure the velocity of the particle during its wrapping process as well as the forces exerted on it by the lipid membrane. Dissipation at the contact line appears to be the main factor determining the wrapping velocity and time to wrap an object.

cond-mat.soft↗

Solid-Liquid Composites for Soft Multifunctional Materials

Soft materials with a liquid component are an emerging paradigm in materials design. The incorporation of a liquid phase, such as water, liquid metals, or complex fluids, into solid materials imparts unique properties and characteristics that emerge as a result of the dramatically different properties of the liquid and solid. Especially in recent years, this has led to the development and study of a range of novel materials with new functional responses, with applications in topics including soft electronics, soft robotics, 3D printing, wet granular systems and even in cell biology. Here we provide a review of solid-liquid composites, broadly defined as a material system with at least one, phase-separated liquid component, and discuss their morphology and fabrication approaches, their emergent mechanical properties and functional response, and the broad range of their applications.

cond-mat.soft↗

Measuring surface tensions of soft solids with huge contact-angle hysteresis

The equilibrium contact angle of a droplet resting on a solid substrate can reveal essential properties of the solid's surface. However, when the motion of a droplet on a surface shows significant hysteresis, it is generally accepted that the solid's equilibrium properties cannot be determined. Here, we describe a method to measure surface tensions of soft solids with strong wetting hysteresis. With independent knowledge of the surface tension of the wetting fluid and the linear-elastic response of the solid, the solid deformations under the contact line and the contact angle of a single droplet together reveal the difference in surface tension of the solid against the liquid and vapor phases. If the solid's elastic properties are unknown, then this surface tension difference can be determined from the change in substrate deformations with contact angle. These results reveal an alternate equilibrium contact angle, equivalent to the classic form of Young-Dupré, but with surface tensions in place of surface energies. We motivate and apply this approach with experiments on gelatin, a common hydrogel.

cond-mat.soft↗

Structural Color from Solid-State Polymerization-Induced Phase Separation

Structural colors are produced by wavelength-dependent scattering of light from nanostructures. While living organisms often exploit phase separation to directly assemble structurally colored materials from macromolecules, synthetic structural colors are typically produced in a two-step process involving the sequential synthesis and assembly of building blocks. Phase separation is attractive for its simplicity, but applications are limited due to a lack of robust methods for its control. A central challenge is to arrest phase separation at the desired length scale. Here, we show that solid-state polymerization-induced phase separation can produce stable structures at optical length scales. In this process, a polymeric solid is swollen and softened with a second monomer. During its polymerization, the two polymers become immiscible and phase separate. As free monomer is depleted, the host matrix resolidifies and arrests coarsening. The resulting PS-PMMA composites have a blue or white appearance. We compare these biomimetic nanostructures to those in structurally-colored feather barbs, and demonstrate the flexibility of this approach by producing structural color in filaments and large sheets.

cond-mat.soft↗

Surface tension and the strain-dependent topography of soft solids

When stretched in one direction, most solids shrink in the transverse directions. In soft silicone gels, however, we observe that small-scale topographical features grow upon stretching. A quantitative analysis of the topography shows that this counter-intuitive response is nearly linear, allowing us to tackle it through a small-strain analysis. We find that the surprising increase of small-scale topography with stretch is due to a delicate interplay of the bulk and surface responses to strain. Specifically, we find that surface tension changes as the material is deformed. This response is expected on general grounds for solid materials, but challenges the standard description of gel- and elastomer-surfaces.

cond-mat.soft↗

Micromirror total internal reflection microscopy for high-performance single particle tracking at interfaces

Single particle tracking has found broad applications in the life and physical sciences, enabling the observation and characterisation of nano- and microscopic motion. Fluorescence-based approaches are ideally suited for high-background environments, such as tracking lipids or proteins in or on cells, due to superior background rejection. Scattering-based detection is preferable when localisation precision and imaging speed are paramount due to the in principle infinite photon budget. Here, we show that micromirror-based total internal reflection dark field microscopy enables background suppression previously only reported for interferometric scattering microscopy, resulting in nm localisation precision at 6 $μ$s exposure time for 20 nm gold nanoparticles with a 25 x 25 $μ$m$^{2}$ field of view. We demonstrate the capabilities of our implementation by characterizing sub-nm deterministic flows of 20 nm gold nanoparticles at liquid-liquid interfaces. Our results approach the optimal combination of background suppression, localisation precision and temporal resolution achievable with pure scattering-based imaging and tracking of nanoparticles at regular interfaces.

physics.optics↗

Droplets sit and slide anisotropically on soft, stretched substrates

Anisotropically wetting substrates enable useful control of droplet behavior across a range of applications. Usually, these involve chemically or physically patterning the substrate surface, or applying gradients in properties like temperature or electrical field. Here, we show that a flat, stretched, uniform soft substrate also exhibits asymmetric wetting, both in terms of how droplets slide and in their static shape. Droplet dynamics are strongly affected by stretch: glycerol droplets on silicone substrates with a 23\% stretch slide 67\% faster in the direction parallel to the applied stretch than in the perpendicular direction. Contrary to classical wetting theory, static droplets in equilibrium appear elongated, oriented parallel to the stretch direction. Both effects arise from droplet-induced deformations of the substrate near the contact line.

cond-mat.soft↗

Viscoelastic and poroelastic relaxations of soft solid surfaces

Understanding surface mechanics of soft solids, such as soft polymeric gels, is crucial in many engineering processes, such as dynamic wetting and adhesive failure. In these situations, a combination of capillary and elastic forces drives the motion, which is balanced by dissipative mechanisms to determine the rate. While shear rheology (i.e. viscoelasticity) has long been assumed to dominate the dissipation, recent works have suggested that compressibility effects (i.e. poroelasticity) could play roles in swollen networks. We use fast interferometric imaging to quantify the relaxation of surface deformations due to a displaced contact line. By systematically measuring the profiles at different time and length scales, we experimentally observe a crossover from viscoelastic to poroelastic surface relaxations.

cond-mat.soft↗

Wrapping of Microparticles by Floppy Lipid Vesicles

Lipid membranes, the barrier defining living cells and many of their sub-compartments, bind to a wide variety of nano- and micro-meter sized objects. In the presence of strong adhesive forces, membranes can strongly deform and wrap the particles, an essential step in crossing the membrane for a variety of health and disease-related processes. A large body of theoretical and numerical work has focused on identifying the physical properties that underly wrapping. Using a model system of micron-sized colloidal particles and giant unilamellar lipid vesicles with tunable adhesive forces, we measure a wrapping phase diagram and make quantitative comparisons to theoretical models. Our data is consistent with a model of membrane-particle interactions accounting for the adhesive energy per unit area, membrane bending rigidity, particle size, and vesicle radius.

cond-mat.soft↗

Surface tensiometry of phase separated protein and polymer droplets by the sessile drop method

Phase separated macromolecules play essential roles in many biological and synthetic systems. Physical characterization of these systems can be challenging because of limited sample volumes, particularly for phase-separated proteins. Here, we demonstrate that a classic method for measuring the surface tension of liquid droplets, based on the analysis of the shape of a sessile droplet, can be effectively scaled down for this application. The connection between droplet shape and surface tension relies on the density difference between the droplet and its surroundings. This can be determined with small sample volumes in the same setup by measuring the droplet sedimentation velocity. An interactive MATLAB script for extracting the capillary length from a droplet image is included in the ESI.

cond-mat.soft↗

Switchable Adhesion of Soft Composites Induced by a Magnetic Field

Switchable adhesives have the potential to improve the manufacturing and recycling of parts and to enable new modes of motility for soft robots. Here, we demonstrate magnetically-switchable adhesion of a two-phase composite to non-magnetic objects. The composite's continuous phase is a silicone elastomer, and the dispersed phase is a magneto-rheological fluid. The composite is simple to prepare, and to mould to different shapes. When a magnetic field is applied, the magneto-rheological fluid develops a yield stress, which dramatically enhances the composite's adhesive properties. We demonstrate up to a nine-fold increase of the pull-off force of non-magnetic objects in the presence of a 250 mT field.

physics.app-ph↗

Elastic stresses reverse Ostwald ripening

When liquid droplets nucleate and grow in a polymer network, compressive stresses can significantly increase their internal pressure, reaching values that far exceed the Laplace pressure. When droplets have grown in a polymer network with a stiffness gradient, droplets in relatively stiff regions of the network tend to dissolve, favoring growth of droplets in softer regions. Here, we show that this elastic ripening can be strong enough to reverse the direction of Ostwald ripening: large droplets can shrink to feed the growth of smaller ones. To numerically model these experiments, we generalize the theory of elastic ripening to account for gradients in solubility alongside gradients in mechanical stiffness.

cond-mat.soft↗

Elastic ripening and inhibition of liquid-liquid phase separation

Phase separation has recently emerged as an important organizational principle in the dense and heterogeneous environment within living cells. Here, we use a synthetic system to show that compressive stresses in a polymer network suppress phase separation of the solvent that swells it. These stresses create a barrier to droplet nucleation that leads to robust, stabilized mixtures well beyond the liquid-liquid phase separation boundary. Network stresses not only alter the stability of mixtures, but they also have a dramatic effect on the ripening of droplets. Gradients in network stresses can drive a new form of ripening, where solute is transported down stiffness gradients. This elastic ripening can be much faster than conventional surface tension driven Ostwald ripening.

cond-mat.soft↗

Extreme cavity expansion in soft solids: damage without fracture

Cavitation is a common damage mechanism in soft solids. Here, we study this using a phase-separation technique in stretched, elastic solids to controllably nucleate and grow small cavities by several orders of magnitude. The ability to make stable cavities of different sizes, as well as the huge range of accessible strains, allows us to systematically study the early stages of cavity expansion. Cavities grow in a scale-free manner, accompanied by irreversible bond breakage that is distributed around the growing cavity, rather than being localized to a crack tip. Furthermore, cavities appear to grow at constant driving pressure. This has strong analogies with the plasticity that occurs surrounding a growing void in ductile metals. In particular we find that, although elastomers are normally considered as brittle materials, small-scale cavity expansion is more like a ductile process. Our results have broad implications for understanding and controlling failure in soft solids.

cond-mat.soft↗

Singular dynamics in the failure of soft adhesive contacts

We characterize the mechanical recovery of compliant silicone gels following adhesive contact failure. We establish broad, stable adhesive contacts between rigid microspheres and soft gels, then stretch the gels to large deformations by pulling quasi-statically on the contact. Eventually, the adhesive contact begins to fail, and ultimately slides to a final contact point on the bottom of the sphere. Immediately after detachment, the gel recoils quickly with a self-similar surface profile that evolves as a power law in time, suggesting that the adhesive detachment point is singular. The singular dynamics we observe are consistent with a relaxation process driven by surface stress and slowed by viscous flow through the porous, elastic network of the gel. Our results emphasize the importance of accounting for both the liquid and solid phases of gels in understanding their mechanics, especially under extreme deformation.

cond-mat.soft↗

The mechanical equilibrium of soft solids with surface elasticity

Recent experiments have shown that surface stresses in soft materials can have a significant strain-dependence. Here we explore the implications of this surface elasticity to show how, and when, we expect it to arise. We develop the appropriate boundary condition, showing that it simplifies significantly in certain cases. We show that surface elasticity's main role is to effectively stiffen a solid surface's response to in-plane tractions, in particular at length-scales smaller than a characteristic elastocapillary length. We also investigate how surface elasticity effects the Green's-function problem of a line force on a flat, linear-elastic substrate. There are significant changes to this solution, especially in that the well-known displacement singularity is regularised. This raises interesting implications for soft phenomena like wetting contact lines, adhesion and friction. Finally, we discuss open questions, future directions, and close ties with existing fields of research.

cond-mat.soft↗

Surface Elastic Constants of a Soft Solid

Solid interfaces have intrinsic elasticity. However, in most experiments, this is obscured by bulk stresses. Through microscopic observations of the contact-line geometry of a partially wetting droplet on an anisotropically stretched substrate, we measure two surface-elastic constants that quantify the linear dependence of the surface stress of a soft polymer gel on its strain. With these two parameters, one can predict surface stresses for general deformations of the material in the linear-elastic limit.

cond-mat.soft↗