arXiv subjects

Robert W. Style

Publications and source records attributed to Robert W. Style.

At least 19 recordsLinked to original sources

arXiv2026

IceCAPA: patterning particles and microorganisms at a freezing front

The ability to precisely pattern micro- and nano-scale objects on surfaces is important for a range of different applications. For example, colloidal patterning has been used to create plasmonic surfaces, light-emitting diodes or authentication marks, while microbial cell patterning can be applied to screening antibiotic response and cellular interactions over larger populations at the single-cell level. However, we still lack versatile techniques that can pattern a wide range of synthetic and biological objects on a spectrum of different substrate types. Here, we present a robust patterning technique based on the directional freezing of a particle or bacterial suspension over a patterned substrate. Growing ice pushes the desired objects into traps in the substrate, while sweeping away non-trapped ones, leaving behind high-fidelity patterns. We show that this method works for a range of different materials (both synthetic particles and microbial cells), and is unaffected by substrate wettability. Furthermore, patterned bacterial cells retain excellent post-assembly viability, highlighting the gentle nature of the assembly technique. Beyond patterning applications, our results also give insights into processes involving the freezing of particulate suspensions. In particular, we demonstrate the importance of the temperature gradient as a key control which determines how particles interact with freezing fronts. Finally, we highlight a tight analogy between particles interacting with a freezing front and with air-water interfaces, suggesting that results from capillarity may shed light on freezing phenomena.

cond-mat.soft↗

arXiv2026

Label-free quantitative imaging of two-dimensional concentration gradients using Fabry-P\'erot interferometry

Concentration gradients at the microscale play a central role in many physical, chemical, and biological systems, yet their quantitative visualization remains challenging due to the limited optical contrast associated with changes in concentration. Here, we present RIO (the Refractive Index Observer), a label-free interferometric tool for quantitative imaging of refractive index, and thus concentration fields in microfluidic systems. Implemented using a Fabry-P\'{e}rot microfluidic chip mounted on a standard optical microscope, RIO achieves a per-pixel refractive index precision on the order of $1\times 10^{-5}$ refractive index units (RIU) using a standard CMOS camera, enabling high sensitivity two-dimensional chemical imaging. We Characterize the refractive index resolution and spatiotemporal performance of the instrument and demonstrate its capabilities by measuring concentration gradients of dissolved NaCl in a co-laminar flow. RIO provides an accessible, label-free platform for quantitative studies of microscale concentration fields in systems where molecular labeling is undesirable or impractical, and enables investigations of a broad range of out-of-equilibrium phenomena, from polymerization and enzymatic reactions to cell signaling and electrochemical processes.

physics.optics↗

arXiv2025

Controlling polymerization-induced phase separation in the synthesis of porous gels

Porous gels -- gels with solvent-filled pores that are much larger than their mesh size -- are widely used in engineering and biomedical applications due to their tunable mechanics, high water content, and selective permeability. Among various strategies to create porous gels, polymerization-induced phase separation (PIPS) has shown particular promise. However, the conditions that trigger and control PIPS remain poorly understood. Here, we systematically investigate the influence of solvent quality, polymeric precursor molecular weight, and polymer concentration on phase separation in polymerizing poly(ethylene glycol) diacrylate gels. We find that phase separation occurs when the precursor solution concentration is below the overlap concentration. Phase-separated gels have a pore geometry that is controlled by solvent quality: better solvents result in smaller pores, while worse solvents can create superporous, highly-absorbant gels. Motivated by our results, we propose a theory that predicts when phase separation occurs in polymerizing gels, applicable across a wide range of polymer/solvent gel systems. Our results provide a framework for the rational design of porous gels.

cond-mat.soft↗

arXiv2025

Thermodynamics of microphase separation in a swollen, strain-stiffening polymer network

Elastic MicroPhase Separation (EMPS) provides a simple route to create soft materials with homogeneous microstructures by leveraging the supersaturation of crosslinked polymer networks with liquids. At low supersaturation, network elasticity stabilizes a uniform mixture, but beyond a critical threshold, metastable microphase-separated domains emerge. While previous theories have focused on describing qualitative features about the size and morphology of these domains, they do not make quantitative predictions about EMPS phase diagrams. In this work, we extend Flory-Huggins theory to quantitatively capture EMPS phase diagrams by incorporating strain-stiffening effects. This model requires no fitting parameters and relies solely on independently measured solubility parameters and large-deformation mechanical responses. Our results reveal that strain-stiffening enables metastable microphase separation within the swelling equilibrium state and why the microstructures can range from discrete droplets to bicontinuous networks. This works highlights the critical role of nonlinear elasticity in controlling phase-separated morphologies in polymer gels.

cond-mat.soft↗

arXiv2024

Sliding or Rolling? Characterizing single-particle contacts

Contacts between particles in dense, sheared suspensions are believed to underpin much of their rheology. Roughness and adhesion are known to constrain the relative motion of particles, and thus globally affect the shear response, but an experimental description of how they microscopically influence the transmission of forces and relative displacements within contacts is lacking. Here we show that an innovative colloidal-probe atomic force microscopy technique allows the simultaneous measurement of normal and tangential forces exchanged between tailored surfaces and microparticles while tracking their relative sliding and rolling, unlocking the direct measurement of coefficients of rolling friction, as well as of sliding friction. We demonstrate that, in the presence of sufficient traction, particles spontaneously roll, reducing dissipation and promoting longer-lasting contacts. Conversely, when rolling is prevented, friction is greatly enhanced for rough and adhesive surfaces, while smooth particles coated by polymer brushes maintain well-lubricated contacts. We find that surface roughness induces rolling due to load-dependent asperity interlocking, leading to large off-axis particle rotations. In contrast, smooth, adhesive surfaces promote rolling along the principal axis of motion. Our results offer direct values of friction coefficients for numerical studies and an interpretation of the onset of discontinuous shear thickening based on them, opening up new ways to tailor rheology via contact engineering.

cond-mat.soft↗

arXiv2024

Unravelling the multiscale surface mechanics of soft solids

Soft solids and their surface deformations control the response of many natural and artificial systems. Yet, their underlying properties are vigorously debated, particularly for polymer networks. While molecular-scale theories predict no interfacial changes with macroscopic deformation, multiple experiments suggest otherwise. To settle this issue, we measure displacement fields near the interface of a silicone gel, in the limit of small deformations. We discover an unexpected multiscale response. The shear modulus decreases smoothly by half with 20 microns of the interface. At the same time we observe a surface excess elasticity, that depends on history and outer medium composition. These results reveal the fundamentally multiscale nature of polymeric surfaces, and call for further experimental and theoretical investigations into the basic understanding of soft solid interfaces

cond-mat.soft↗

arXiv2024

Droplets sliding on soft solids shed elastocapillary rails

The surface tension of partially wetting droplets deforms soft substrates. These deformations are usually localized to a narrow region near the contact line, forming a so-called `elastocapillary ridge.' When a droplet slides along a substrate, the movement of the elastocapillary ridge dissipates energy in the substrate and slows the droplet down. Previous studies have analyzed isotropically spreading droplets and found that the advancing contact line `surfs' the elastocapillary ridge, with a velocity determined by a local balance of capillary forces and bulk rheology. Here, we experimentally explore the dynamics of a droplet sliding across soft substrates. At low velocities, the contact line is nearly circular, and dissipation increases logarithmically with speed. At higher droplet velocities, the contact line adopts a bullet-like shape, and the dissipation levels off. At the same time, droplets shed a pair of `elastocapillary rails' that fade away slowly behind it. These results suggest that droplets favor sliding along a stationary ridge over surfing atop a translating one.

cond-mat.soft↗

arXiv2024

Characterizing hydrogel behavior under compression with gel-freezing osmometry

Hydrogels are particularly versatile materials that are widely found in both Nature and industry. One key reason for this versatility is their high water content, which lets them dramatically change their volume and many of their mechanical properties -- often by orders of magnitude -- as they swell and dry out. Currently, we lack techniques that can precisely characterize how these properties change with water content. To overcome this challenge, here we develop Gel-Freezing Osmometry (GelFrO): an extension of freezing-point osmometry. We show how GelFrO can measure a hydrogel's mechanical response to compression and osmotic pressure, while only using small, $O(100μ$L$)$ samples. Because the technique allows measurement of properties over an unusually wide range of water contents, it allows us to accurately test theoretical predictions. We find simple, power-law behavior for both mechanical response to compression, and osmotic pressure, while these are not well-captured by classical Flory-Huggins theory. We interpret this power-law behavior as a hallmark of a microscopic fractal structure of the gel's polymer network, and propose a simple way to connect the gel's fractal dimension to its mechanical and osmotic properties. This connection is supported by observations of hydrogel microstructures using small-angle x-ray scattering. Finally, our results motivate us to propose an updated constitutive model describing hydrogel swelling, and mechanical response.

cond-mat.soft↗

arXiv2024

Dehydration drives damage in the freezing of brittle hydrogels

It is widely known that freezing breaks soft, wet materials. However, the mechanism underlying this damage is still not clear. To understand this process, we freeze model, brittle hydrogel samples, while observing the growth of ice-filled cracks that break these apart. We show that damage is not caused by the expansion of water upon freezing, or the growth of ice-filled cavities in the hydrogel. Instead, local ice growth dehydrates the surrounding hydrogel, leading to drying-induced fracture. This dehydration is driven by the process of cryosuction, whereby undercooled ice sucks nearby water towards itself, feeding its growth. Our results highlight the strong analogy between freezing damage and desiccation cracking, which we anticipate being useful for developing an understanding of both topics. Our results should also give useful insights into a wide range of freezing processes, including cryopreservation, food science and frost heave.

cond-mat.soft↗

arXiv2023

Polycrystallinity enhances stress build-up around ice

Damage caused by freezing wet, porous materials is a widespread problem, but is hard to predict or control. Here, we show that polycrystallinity makes a great difference to the stress build-up process that underpins this damage. Unfrozen water in grain-boundary grooves feeds ice growth at temperatures below the freezing temperature, leading to the fast build-up of localized stresses. The process is very variable, which we ascribe to local differences in ice-grain orientation, and to the surprising mobility of many grooves -- which further accelerates stress build-up. Our work will help understand how freezing damage occurs, and in developing accurate models and effective damage-mitigation strategies.

cond-mat.soft↗

arXiv2023

Strain-stiffening elastomers fail from the edge

The accurate measurement of fracture resistance in elastomers is essential for predicting the mechanical limits of soft devices. Usually, this is achieved by performing tearing or peeling experiments on thin-sheet samples. Here, we show that these tests can be surprisingly thickness-dependent, with thicker samples being significantly stronger than thinner ones. Even for a simple geometry, direct imaging of the fracture surface shows that the fracture process actually involves three distinct cracks: an inner crack, and two edge cracks. Ultimately, samples fail when two edge cracks meet at the sample's mid-plane. The opening angle of edge crack, $2 θ$, determines how far the sample has to be stretched before the edge cracks meet. Conveniently, $θ$ is a material property that can be inferred from the elastomer's non-linear elastic response. To yield thickness-independent fracture-test results, sample thickness should be much smaller than the smallest lateral sample dimension divided by $\tan θ$. Our results have direct implications for characterizing, understanding, and modelling fracture in soft elastomers.

cond-mat.soft↗

arXiv2023

Surface Passivation Method for Super-repellence of Aqueous Macromolecular Condensates

Solutions of macromolecules can undergo liquid-liquid phase separation to form droplets with ultra-low surface tension. Droplets with such low surface tension wet and spread over common surfaces such as test tubes and microscope slides, complicating \textit{in vitro} experiments. Development of an universal super-repellent surface for macromolecular droplets has remained elusive because their ultra-low surface tension requires low surface energies. Furthermore, 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 $θ\approx180^\circ)$ and minimal pinning of phase-separated droplets in aqueous solution. The hydrogel is based on a swollen matrix of chemically crosslinked polyethylene glycol diacrylate of molecular weight 12 kDa (PEGDA), and can be prepared with basic chemistry lab equipment. The PEGDA hydrogel is a powerful tool for \textit{in vitro} studies of weak interactions, dynamics, and internal organization of phase-separated droplets in aqueous solutions.

cond-mat.soft↗

arXiv2023

Elastic Microphase Separation Produces Robust Bicontinuous Materials

Bicontinuous microstructures are essential to the function of diverse natural and synthetic systems. Their synthesis has been based on two approaches: arrested phase separation or self-assembly of block copolymers. The former is attractive for its chemical simplicity, the latter for its thermodynamic robustness. Here, we introduce Elastic MicroPhase Separation (EMPS) as an alternative approach to make bicontinuous microstructures. Conceptually, EMPS balances the molecular-scale forces that drive demixing with large-scale elasticity to encode a thermodynamic length scale. This process features a continuous phase transition, reversible without hysteresis. Practically, we trigger EMPS by simply super-saturating an elastomeric matrix with a liquid. This results in uniform bicontinuous materials with a well-defined microscopic length-scale tuned by the matrix stiffness. The versatility and robustness of EMPS is further demonstrated by fabricating bicontinuous materials with superior mechanical properties and controlled anisotropy and microstructural gradients.

cond-mat.soft↗

arXiv2023

The generalized Clapeyron equation and its application to confined ice growth

Most theoretical descriptions of stresses induced by freezing are rooted in the (generalized) Clapeyron equation, which predicts the pressure that a solid can exert as it cools below its melting temperature. This equation is central for topics ranging beyond glaciology to geomorphology, civil engineering, food storage, and cryopreservation. However, it has inherent limitations, requiring isotropic solid stresses and conditions near bulk equilibrium. Here, we examine when the Clapeyron equation is applicable by providing a rigorous derivation that details all assumptions. We demonstrate the natural extension for anisotropic stress states, and we show how the temperature and pressure ranges for validity depend on well-defined material properties. Finally, we demonstrate how the range of applicability of the (linear) Clapeyron equation can be extended by adding higher-order terms, yielding results that are in good agreement with experimental data for the pressure melting of ice.

cond-mat.soft↗

arXiv2022

Gradients in solid surface tension drive Marangoni-like motions in cell aggregates

The surface tension of living cells and tissues originates from the generation of nonequilibrium active stresses within the cell cytoskeleton. Here, using laser ablation, we generate gradients in the surface tension of cellular aggregates as models of simple tissues. These gradients of active surface stress drive large-scale and rapid toroidal motion. Subsequently, the motions spontaneously reverse as stresses reaccumulate and cells return to their original positions. Both forward and reverse motions resemble Marangoni flows in viscous fluids. However, the motions are faster than the timescales of viscoelastic relaxation, and the surface tension gradient is proportional to mechanical strain at the surface. Further, due to active stress, both the surface tension gradient and surface strain are dependent upon the volume of the aggregate. These results indicate that surface tension can induce rapid and highly correlated elastic deformations in the maintenance of tissue shape and configuration.

physics.bio-ph↗

arXiv2022

Hydroelastomers: soft, tough, highly swelling composites

Inspired by the cellular design of plant tissue, we present a new approach to make versatile, tough, highly water-swelling composites. We embed highly swelling hydrogel particles inside tough, water-permeable, elastomeric matrices. The resulting composites, which we call \emph{hydroelastomers}, show little softening as they swell, and have excellent fracture properties that match those of the best-performing, tough hydrogels. Our composites are straightforward to fabricate, based on commercial materials, and can easily be molded or extruded to form shapes with complex swelling geometries. Furthermore, there is a large design space available for making hydroelastomers, since one can use any hydrogel as the dispersed phase in the composite, including hydrogels with stimuli-responsiveness. These features should make hydroelastomers excellent candidates for use in soft robotics and swelling-based actuation, or as shape-morphing materials, while also being useful as hydrogel replacements in a wide range of other fields.

cond-mat.soft↗

arXiv2021

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↗

arXiv2021

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↗