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Showing papers in "Soft Matter in 2015"


Journal ArticleDOI
TL;DR: This paper provides a concise and comprehensive review of Pickering emulsion systems that possess the ability to respond to an array of external triggers, including pH, temperature, CO2 concentration, light intensity, ionic strength, and magnetic field.
Abstract: Pickering emulsions possess many advantages over traditional surfactant stabilized emulsions. For example, Pickering emulsions impart better stability against coalescence and, in many cases, are biologically compatible and environmentally friendly. These characteristics open the door for their use in a variety of industries spanning petroleum, food, biomedicine, pharmaceuticals, and cosmetics. Depending on the application, rapid, but controlled stabilization and destabilization of an emulsion may be necessary. As a result, Pickering emulsions with stimuli-responsive properties have, in recent years, received a considerable amounts of attention. This paper provides a concise and comprehensive review of Pickering emulsion systems that possess the ability to respond to an array of external triggers, including pH, temperature, CO2 concentration, light intensity, ionic strength, and magnetic field. Potential applications for which stimuli-responsive Pickering emulsion systems would be of particular value, such as emulsion polymerization, enhanced oil recovery, catalyst recovery, and cosmetics, are discussed.

453 citations


Journal ArticleDOI
TL;DR: This work image the shape of drops on lubricant-infused surfaces by laser scanning confocal microscopy and reveals fundamentally different processes at the front and rear of moving drops.
Abstract: For a liquid droplet to slide down a solid planar surface, the surface usually has to be tilted above a critical angle of approximately 10°. By contrast, droplets of nearly any liquid “slip” on lubricant-infused textured surfaces – so termed slippery surfaces – when tilted by only a few degrees. The mechanism of how the lubricant alters the static and dynamic properties of the drop remains elusive because the drop–lubricant interface is hidden. Here, we image the shape of drops on lubricant-infused surfaces by laser scanning confocal microscopy. The contact angle of the drop–lubricant interface with the substrate exceeds 140°, although macroscopic contour images suggest angles as low as 60°. Confocal microscopy of moving drops reveals fundamentally different processes at the front and rear. Drops recede via discrete depinning events from surface protrusions at a defined receding contact angle, whereas the advancing contact angle is 180°. Drops slide easily, as the apparent contact angles with the substrate are high and the drop–lubricant interfacial tension is typically lower than the drop–air interfacial tension. Slippery surfaces resemble superhydrophobic surfaces with two main differences: drops on a slippery surface are surrounded by a wetting ridge of adjustable height and the air underneath the drop in the case of a superhydrophobic surface is replaced by lubricant in the case of a slippery surface.

318 citations


Journal ArticleDOI
TL;DR: This work predicts that near a hard planar wall such a Janus particle exhibits several scenarios of motion, and proposes that a desired behavior can be selected by tuning these parameters via a judicious design of the particle surface chemistry.
Abstract: Micron-sized particles moving through a solution in response to self-generated chemical gradients serve as model systems for studying active matter. Their far-reaching potential applications will require the particles to sense and respond to their local environment in a robust manner. The self-generated hydrodynamic and chemical fields, which induce particle motion, probe and are modified by that very environment, including confining boundaries. Focusing on a catalytically active Janus particle as a paradigmatic example, we predict that near a hard planar wall such a particle exhibits several scenarios of motion: reflection from the wall, motion at a steady-state orientation and height above the wall, or motionless, steady “hovering.” Concerning the steady states, the height and the orientation are determined both by the proportion of catalyst coverage and the interactions of the solutes with the different “faces” of the particle. Accordingly, we propose that a desired behavior can be selected by tuning these parameters via a judicious design of the particle surface chemistry.

225 citations


Journal ArticleDOI
TL;DR: Conceptual similarities to superhydrophobic surfaces, capillary origami, slippery liquids-infused porous surfaces (SLIPS) and Leidenfrost droplets are discussed and applications including detecting changes in physical properties are described.
Abstract: The study of particle stabilized interfaces has a long history in terms of emulsions, foams and related dry powders. The same underlying interfacial energy principles also allow hydrophobic particles to encapsulate individual droplets into a stable form as individual macroscopic objects, which have recently been called “Liquid Marbles”. Here we discuss conceptual similarities to superhydrophobic surfaces, capillary origami, slippery liquids-infused porous surfaces (SLIPS) and Leidenfrost droplets. We provide a review of recent progress on liquid marbles, since our earlier Emerging Area article (Soft Matter, 2011, 7, 5473–5481), and speculate on possible future directions from new liquid-infused liquid marbles to microarray applications. We highlight a range of properties of liquid marbles and describe applications including detecting changes in physical properties (e.g. pH, UV, NIR, temperature), use for gas sensing, synthesis of compounds/composites, blood typing and cell culture.

197 citations


Journal ArticleDOI
TL;DR: The first time-resolved experimental investigation of microdroplet impact at velocities up to V0 = 50 m s(-1), on hydrophilic and -phobic surfaces at frame rates exceeding 10(7) frames per second confirms that the ambient gas properties are key ingredients for splash threshold predictions.
Abstract: Technologies including (3D-) (bio-)printing, diesel engines, laser-induced forward transfer, and spray cleaning require optimization and therefore understanding of micrometer-sized droplets impacting at velocities beyond 10 m s−1. However, as yet, this regime has hardly been addressed. Here we present the first time-resolved experimental investigation of microdroplet impact at velocities up to V0 = 50 m s−1, on hydrophilic and -phobic surfaces at frame rates exceeding 107 frames per second. A novel method to determine the 3D-droplet profile at sub-micron resolution at the same frame rates is presented, using the fringe pattern observed from a bottom view. A numerical model, which is validated by the side- and bottom-view measurements, is employed to study the viscous boundary layer inside the droplet and the development of the rim. The spreading dynamics, the maximal spreading diameter, the boundary layer thickness, the rim formation, and the air bubble entrainment are compared to theory and previous experiments. In general, the impact dynamics are equal to millimeter-sized droplet impact for equal Reynolds-, Weber- and Stokes numbers (Re, We, and St, respectively). Using our numerical model, effective scaling laws for the progression of the boundary layer thickness and the rim diameter are provided. The dimensionless boundary layer thickness develops in time (t) according to , and the diameter of the rim develops as , with drop diameter D0 and inertial time scale τ = D0/V0. These scalings differ from previously assumed, but never validated, values. Finally, no splash is observed, at variance with many predictions but in agreement with models including the influence of the surrounding gas. This confirms that the ambient gas properties are key ingredients for splash threshold predictions.

177 citations


Journal ArticleDOI
TL;DR: This work focuses in particular on how the jammed aggregate state can be tailored by controlling particle level properties and discusses very recent ideas that provide an important first step toward actual design of specifically targeted jamming behavior.
Abstract: In materials science, high performance is typically associated with regularity and order, while disorder and the presence of defects are assumed to lead to sub-optimal outcomes. This holds for traditional solids such as crystals as well as for many types of nanoscale devices. However, there are circumstances where disorder can be harnessed to achieve performance not possible with approaches based on regularity. Recent research has shown opportunities specifically for soft matter. There, the phenomenon of jamming leads to unique emergent behavior that enables disordered, amorphous systems to switch reversibly between solid-like rigidity and fluid-like plasticity. This makes it possible to envision materials that can change stiffness or even shape adaptively. We review some of the progress in this direction, discussing examples where jamming has been explored from micro to macro scales in colloidal systems, suspensions, granular-materials-enabled soft robotics, and architecture. We focus in particular on how the jammed aggregate state can be tailored by controlling particle level properties and discuss very recent ideas that provide an important first step toward actual design of specifically targeted jamming behavior.

176 citations


Journal ArticleDOI
TL;DR: Red light irradiation induced a gel-to-sol transition as a result of the disassembly of the mAzo/β-CD complexes, which could control protein release from the hydrogel in tissue due to its deep penetration depth in tissue.
Abstract: We report a novel red-light-responsive supramolecule. The tetra-ortho-methoxy-substituted azobenzene (mAzo) and β-cyclodextrin (β-CD) spontaneously formed a supramolecular complex. The substituted methoxy groups shifted the responsive wavelength of the azo group to the red light region, which is in the therapeutic window and desirable for biomedical applications. Red light induced the isomerization of mAzo and the disassembly of the mAzo/β-CD supramolecular complex. We synthesized a mAzo-functionalized polymer and a β-CD-functionalized polymer. Mixing the two polymers in an aqueous solution generated a supramolecular hydrogel. Red light irradiation induced a gel-to-sol transition as a result of the disassembly of the mAzo/β-CD complexes. Proteins were loaded in the hydrogel. Red light could control protein release from the hydrogel in tissue due to its deep penetration depth in tissue. We envision the use of red-light-responsive supramolecules for deep-tissue biomedical applications.

157 citations


Journal ArticleDOI
TL;DR: Besides the surface roughness structure, the high fluoride enrichment on the surface plays a major role in the superhydrophobic and anti-icing properties under overcooled conditions.
Abstract: A superhydrophobic surface with anti-icing performance has been the focus of research, but few studies have reported the effective and low cost strategy that met the requirements under overcooled conditions. In this article, the fluorinated sol-gel colloid coatings were simply prepared via hydrolytic condensation of nanosilica sol, methyltriethoxysilane (MTES) and 3-[(perfluorohexylsulfonyl)amino]propyltriethoxysilane (HFTES). The multi scale morphology and chemical composition of the artificial surfaces were characterized by scanning electron microscopy (SEM), atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS). The influence of the surface roughness structure and fluorinated groups on the wettability and freezing delay time of the colloid surface under overcooled conditions were explored. As the HFTES content was higher than 6 wt%, the prepared colloid surface showed excellent superhydropobicity with a contact angle (CA) of about 166° at room temperature. The CA gradually reduced with the decrease of the temperature. Only the samples with high HFTES contents (above 30 wt%) exhibited special superhydrophobic and anti-icing properties under freeze temperature. Besides the surface roughness structure, the high fluoride enrichment on the surface plays a major role in the superhydrophobic and anti-icing properties under overcooled conditions.

153 citations


Journal ArticleDOI
TL;DR: Self-healing oxime-functional hydrogels have been developed that undergo a reversible gel-to-sol transition via oxime exchange under acidic conditions and can either form dynamic-covalent or physically-crosslinked gels, both of which demonstrate reversible gelation behavior.
Abstract: Self-healing oxime-functional hydrogels have been developed that undergo a reversible gel-to-sol transition via oxime exchange under acidic conditions. Keto-functional copolymers were prepared by conventional radical polymerization of N,N-dimethylacrylamide (DMA) and diacetone acrylamide (DAA). The resulting water soluble copolymers (P(DMA-stat-DAA)) were chemically crosslinked with difunctional alkoxyamines to obtain hydrogels via oxime formation. Gel-to-sol transitions were induced by the addition of excess monofunctional alkoxyamines to promote competitive oxime exchange under acidic conditions at 25 °C. The hydrogel could autonomously heal after it was damaged due to the dynamic nature of the oxime crosslinks. In addition to their chemo-responsive behavior, the P(DMA-stat-DAA) copolymers exhibit cloud points which vary with the DAA content in the copolymers. This thermo-responsive behavior of the P(DMA-stat-DAA) was utilized to form physical hydrogels above their cloud point. Therefore, these materials can either form dynamic-covalent or physically-crosslinked gels, both of which demonstrate reversible gelation behavior.

149 citations


Journal ArticleDOI
TL;DR: A self-healable polymeric hydrogel consisting of biocompatible and biodegradable polysaccharides can be applied to various biomedical fields by self-crosslinking two natural polymers acrylamide-modified chitin containing amino groups and oxidized alginate containing dialdehyde groups.
Abstract: Natural polymeric hydrogels with self-healing capability that can recover the functionalities and structures of gels after damage are extremely attractive due to their emerging applications in the biomedical field. Here we report a self-healable polymeric hydrogel by self-crosslinking two natural polymers acrylamide-modified chitin (AMC) containing amino groups and oxidized alginate containing dialdehyde groups. The generation of the self-crosslinked hydrogel relies on the dynamic covalent linkage through Schiff base between the polysaccharide chains. The self-healing capability of the crosslinked hydrogel depends on the molar ratio of AMC and oxidized alginate and the surrounding pH. Under certain circumstances, the damaged hydrogel shows a complete recovery and can be stretched to a favorable extent, which is seldom observed for polysaccharide self-healing hydrogel. Notably, we find that the self-healing ability can be “stored” by freeze-drying and “activated” by rehydration. In addition, we demonstrate that the hydrogel can be used as a soft template to guide the repair of inorganic materials like hydroxyapatite. We anticipate that this self-healable hydrogel consisting of biocompatible and biodegradable polysaccharides can be applied to various biomedical fields.

148 citations


Journal ArticleDOI
TL;DR: The pressure of suspensions of self-propelled objects is studied theoretically and by simulation of spherical active Brownian particles (ABPs) to show that for certain geometries, the mechanical pressure as force/area of confined systems can be equally expressed by bulk properties, which implies the existence of a nonequilibrium equation of state.
Abstract: The pressure of suspensions of self-propelled objects is studied theoretically and by simulation of spherical active Brownian particles (ABPs). We show that for certain geometries, the mechanical pressure as force/area of confined systems can be equally expressed by bulk properties, which implies the existence of a nonequilibrium equation of state. Exploiting the virial theorem, we derive expressions for the pressure of ABPs confined by solid walls or exposed to periodic boundary conditions. In both cases, the pressure comprises three contributions: the ideal-gas pressure due to white-noise random forces, an activity-induced pressure (“swim pressure”), which can be expressed in terms of a product of the bare and a mean effective particle velocity, and the contribution by interparticle forces. We find that the pressure of spherical ABPs in confined systems explicitly depends on the presence of the confining walls and the particle–wall interactions, which has no correspondence in systems with periodic boundary conditions. Our simulations of three-dimensional ABPs in systems with periodic boundary conditions reveal a pressure–concentration dependence that becomes increasingly nonmonotonic with increasing activity. Above a critical activity and ABP concentration, a phase transition occurs, which is reflected in a rapid and steep change of the pressure. We present and discuss the pressure for various activities and analyse the contributions of the individual pressure components.

Journal ArticleDOI
TL;DR: The design rationale for the creation of ionic cross-linked hydrogels is to graft an acrylic acid monomer on the surface of vinyl hybrid silica nanoparticles for the growth of poly(acrylic) acid (PAA), and the obtained VSNP-PAA nanobrush can be used as a gelator.
Abstract: We present a facile strategy to synthesize self-healable tough and highly stretchable hydrogels. Our design rationale for the creation of ionic cross-linked hydrogels is to graft an acrylic acid monomer on the surface of vinyl hybrid silica nanoparticles (VSNPs) for the growth of poly(acrylic) acid (PAA), and the obtained VSNP–PAA nanobrush can be used as a gelator. Physical cross-linking through hydrogen bonding and ferric ion-mediated ionic interactions between PAA polymer chains of the gelators yielded ionic nanocomposite physical hydrogels with excellent and balanced mechanical properties (tensile strength 860 kPa, elongation at break ∼2300%), and the ability to self-repair (tensile strength ∼560 kPa, elongation at break ∼1800%). The toughness and stretchability arise from the reversible cross-linking interactions between the polymer chains that help dissipate energy through stress (deformation) triggered dynamic processes. These unique properties will enable greater application of these hydrogel materials, especially in tissue engineering.

Journal ArticleDOI
TL;DR: The developed force clamp force mapping (FCFM), an atomic force microscopy technique for measuring the viscoelastic creep behavior of live cells with sub-micrometer spatial resolution, can uncover subtle mechanical signatures of proteins in living cells.
Abstract: We developed force clamp force mapping (FCFM), an atomic force microscopy (AFM) technique for measuring the viscoelastic creep behavior of live cells with sub-micrometer spatial resolution. FCFM combines force–distance curves with an added force clamp phase during tip-sample contact. From the creep behavior measured during the force clamp phase, quantitative viscoelastic sample properties are extracted. We validate FCFM on soft polyacrylamide gels. We find that the creep behavior of living cells conforms to a power-law material model. By recording short (50–60 ms) force clamp measurements in rapid succession, we generate, for the first time, two-dimensional maps of power-law exponent and modulus scaling parameter. Although these maps reveal large spatial variations of both parameters across the cell surface, we obtain robust mean values from the several hundreds of measurements performed on each cell. Measurements on mouse embryonic fibroblasts show that the mean power-law exponents and the mean modulus scaling parameters differ greatly among individual cells, but both parameters are highly correlated: stiffer cells consistently show a smaller power-law exponent. This correlation allows us to distinguish between wild-type cells and cells that lack vinculin, a dominant protein of the focal adhesion complex, even though the mean values of viscoelastic properties between wildtype and knockout cells did not differ significantly. Therefore, FCFM spatially resolves viscoelastic sample properties and can uncover subtle mechanical signatures of proteins in living cells.

Journal ArticleDOI
TL;DR: It is shown that due to limits of vapor sorption within a liquid, nucleation is most favoured at the liquid-air interface and that on spreading liquids, droplet submergence within the liquid occurs thereafter and the viscosity of the liquid does not affect droplet nucleation.
Abstract: Condensation on liquids has been studied extensively in context of breath figure templating, materials synthesis and enhancing heat transfer using liquid impregnated surfaces. However, the mechanics of nucleation and growth on liquids remains unclear, especially on liquids that spread on the condensate. By examining the energy barriers of nucleation, we provide a framework to choose liquids that can lead to enhanced nucleation. We show that due to limits of vapor sorption within a liquid, nucleation is most favoured at the liquid–air interface and demonstrate that on spreading liquids, droplet submergence within the liquid occurs thereafter. We provide a direct visualization of the thin liquid profile that cloaks the condensed droplet on a liquid impregnated surface and elucidate the vapour transport mechanism in the liquid films. Finally, we show that although the viscosity of the liquid does not affect droplet nucleation, it plays a crucial role in droplet growth.

Journal ArticleDOI
TL;DR: In this paper, the authors considered the hydrodynamic capture of a microswimmer near a stationary spherical obstacle and provided expressions for the critical trapping radius, the depth of the "basin of attraction", and the scattering angle.
Abstract: Motivated by recent experiments, we consider the hydrodynamic capture of a microswimmer near a stationary spherical obstacle. Simulations of model equations show that a swimmer approaching a small spherical colloid is simply scattered. In contrast, when the colloid is larger than a critical size it acts as a passive trap: the swimmer is hydrodynamically captured along closed trajectories and endlessly orbits around the colloidal sphere. In order to gain physical insight into this hydrodynamic scattering problem, we address it analytically. We provide expressions for the critical trapping radius, the depth of the “basin of attraction,” and the scattering angle, which show excellent agreement with our numerical findings. We also demonstrate and rationalize the strong impact of swimming-flow symmetries on the trapping efficiency. Finally, we give the swimmer an opportunity to escape the colloidal traps by considering the effects of Brownian, or active, diffusion. We show that in some cases the trapping time is governed by an Ornstein–Uhlenbeck process, which results in a trapping time distribution that is well-approximated as inverse-Gaussian. The predictions again compare very favorably with the numerical simulations. We envision applications of the theory to bioremediation, microorganism sorting techniques, and the study of bacterial populations in heterogeneous or porous environments.

Journal ArticleDOI
TL;DR: In this article, a stochastic description of a model of N mutually interacting active particles in the presence of external fields and characterize its steady state behavior in the absence of currents is presented.
Abstract: We present a stochastic description of a model of N mutually interacting active particles in the presence of external fields and characterize its steady state behavior in the absence of currents. To reproduce the effects of the experimentally observed persistence of the trajectories of the active particles we consider a Gaussian force having a non-vanishing correlation time τ, whose finiteness is a measure of the activity of the system. With these ingredients we show that it is possible to develop a statistical mechanical approach similar to the one employed in the study of equilibrium liquids and to obtain the explicit form of the many-particle distribution function by means of the multidimensional unified colored noise approximation. Such a distribution plays a role analogous to the Gibbs distribution in equilibrium statistical mechanics and provides complete information about the microscopic state of the system. From here we develop a method to determine the one- and two-particle distribution functions in the spirit of the Born–Green–Yvon (BGY) equations of equilibrium statistical mechanics. The resulting equations which contain extra-correlations induced by the activity allow us to determine the stationary density profiles in the presence of external fields, the pair correlations and the pressure of active fluids. In the low density regime we obtained the effective pair potential ϕ(r) acting between two isolated particles separated by a distance, r, showing the existence of an effective attraction between them induced by activity. Based on these results, in the second half of the paper we propose a mean field theory as an approach simpler than the BGY hierarchy and use it to derive a van der Waals expression of the equation of state.

Journal ArticleDOI
TL;DR: This article classify the instability of a thin polymer film into three broad categories, which are: instability of an ultra-thin (<100 nm) viscous film engendered by amplification of thermally excited surface capillary waves due to interfacial dispersive van der Waals forces, and instability arising from the attractive inter-surface interactions.
Abstract: The free surface of a thin soft polymer film is often found to become unstable and self-organizes into various meso-scale structures. In this article we classify the instability of a thin polymer film into three broad categories, which are: category 1: instability of an ultra-thin (<100 nm) viscous film engendered by amplification of thermally excited surface capillary waves due to interfacial dispersive van der Waals forces; category 2: instability arising from the attractive inter-surface interactions between the free surface of a soft film exhibiting room temperature elasticity and another rigid surface in its contact proximity; and category 3: instability caused by an externally applied field such as an electric field or a thermal gradient, observed in both viscous and elastic films. We review the salient features of each instability class and highlight how characteristic length scales, feature morphologies, evolution pathways, etc. depend on initial properties such as film thickness, visco-elasticity (rheology), residual stress, and film preparation conditions. We emphasize various possible strategies for aligning and ordering of the otherwise isotropic structures by combining the essential concepts of bottom-up and top-down approaches. A perspective, including a possible future direction of research, novelty and limitations of the methods, particularly in comparison to the existing patterning techniques, is also presented for each setting.

Journal ArticleDOI
TL;DR: This review discusses the theory, synthesis, and applications of PE brushes, and sheds light on the state of the art in continuum modelling approaches for polymer and PE brushes directed towards analysis beyond the scaling calculations.
Abstract: Polyelectrolyte (PE) brushes are a special class of polymer brushes (PBs) containing charges. Polymer chains attain “brush”-like configuration when they are grafted or get localized at an interface (solid–fluid or liquid–fluid) with sufficiently close proximity between two-adjacent grafted polymer chains – such a proximity triggers a particular nature of interaction between the adjacent polymer molecules forcing them to stretch orthogonally to the grafting interface, instead of random-coil arrangement. In this review, we discuss the theory, synthesis, and applications of PE brushes. The theoretical discussion starts with the standard scaling concepts for polymer and PE brushes; following that, we shed light on the state of the art in continuum modelling approaches for polymer and PE brushes directed towards analysis beyond the scaling calculations. A special emphasis is laid in pinpointing the cases for which the PE electrostatic effects can be de-coupled from the PE entropic and excluded volume effects; such de-coupling is necessary to appropriately probe the complicated electrostatic effects arising from pH-dependent charging of the PE brushes and the use of these effects for driving liquid and ion transport at the interfaces covered with PE brushes. We also discuss the atomistic simulation approaches for polymer and PE brushes. Next we provide a detailed review of the existing approaches for the synthesis of polymer and PE brushes on interfaces, nanoparticles, and nanochannels, including mixed brushes and patterned brushes. Finally, we discuss some of the possible applications and future developments of polymer and PE brushes grafted on a variety of interfaces.

Journal ArticleDOI
TL;DR: Insight is provided into how by combining a long history of application, with modern methods of derivatisation and analysis, the future for this family of gelators is bright, with an increasing number of high-tech applications, from environmental remediation to tissue engineering, being within reach.
Abstract: Dibenzylidene-D-sorbitol (DBS) has been a well-known low-molecular-weight gelator of organic solvents for over 100 years. As such, it constitutes a very early example of a supramolecular gel – a research field which has recently developed into one of intense interest. The ability of DBS to self-assemble into sample-spanning networks in numerous solvents is predicated upon its ‘butterfly-like’ structure, whereby the benzylidene groups constitute the ‘wings’ and the sorbitol backbone the ‘body’ – the two parts representing the molecular recognition motifs underpinning its gelation mechanism, with the nature of solvent playing a key role in controlling the precise assembly mode. This gelator has found widespread applications in areas as diverse as personal care products and polymer nucleation/clarification, and has considerable potential in applications such as dental composites, energy technology and liquid crystalline materials. Some derivatives of DBS have also been reported which offer the potential to expand the scope and range of applications of this family of gelators and endow the nansocale network with additional functionality. This review aims to explain current trends in DBS research, and provide insight into how by combining a long history of application, with modern methods of derivatisation and analysis, the future for this family of gelators is bright, with an increasing number of high-tech applications, from environmental remediation to tissue engineering, being within reach.

Journal ArticleDOI
TL;DR: The recently proposed nonlocal granular fluidity model is applied to this geometry and it is found that the model captures many of these effects, including the Froude number of the flows, which has been shown experimentally to collapse.
Abstract: Flows of granular media down a rough inclined plane demonstrate a number of nonlocal phenomena. We apply the recently proposed nonlocal granular fluidity model to this geometry and find that the model captures many of these effects. Utilizing the model's dynamical form, we obtain a formula for the critical stopping height of a layer of grains on an inclined surface. Using an existing parameter calibration for glass beads, the theoretical result compares quantitatively to existing experimental data for glass beads. This provides a stringent test of the model, whose previous validations focused on driven steady-flow problems. For layers thicker than the stopping height, the theoretical flow profiles display a thickness-dependent shape whose features are in agreement with previous discrete particle simulations. We also address the issue of the Froude number of the flows, which has been shown experimentally to collapse as a function of the ratio of layer thickness to stopping height. While the collapse is not obvious, two explanations emerge leading to a revisiting of the history of inertial rheology, which the nonlocal model references for its homogeneous flow response.

Journal ArticleDOI
TL;DR: In this paper, the rotational diffusion coefficient has an activity-induced contribution given by vc/ξP, where vc is the contour velocity and ξP the persistence length.
Abstract: Worm-like filaments that are propelled homogeneously along their tangent vector are studied by Brownian dynamics simulations. Systems in two dimensions are investigated, corresponding to filaments adsorbed to interfaces or surfaces. A large parameter space covering weak and strong propulsion, as well as flexible and stiff filaments is explored. For strongly propelled and flexible filaments, the free-swimming filaments spontaneously form stable spirals. The propulsion force has a strong impact on dynamic properties, such as the rotational and translational mean square displacement and the rate of conformational sampling. In particular, when the active self-propulsion dominates thermal diffusion, but is too weak for spiral formation, the rotational diffusion coefficient has an activity-induced contribution given by vc/ξP, where vc is the contour velocity and ξP the persistence length. In contrast, structural properties are hardly affected by the activity of the system, as long as no spirals form. The model mimics common features of biological systems, such as microtubules and actin filaments on motility assays or slender bacteria, and artificially designed microswimmers.

Journal ArticleDOI
TL;DR: It is found that the TNE strength attains its maximum at the end of the spinodal decomposition stage, and it decreases when the latent heat increases from zero.
Abstract: A discrete Boltzmann model (DBM) is developed to investigate the hydrodynamic and thermodynamic non-equilibrium (TNE) effects in phase separation processes. The interparticle force drives changes and the gradient force, induced by gradients of macroscopic quantities, opposes them. In this paper, we investigate the interplay between them by providing a detailed inspection of various non-equilibrium observables. Based on the TNE features, we define TNE strength which roughly estimates the deviation amplitude from the thermodynamic equilibrium. The time evolution of the TNE intensity provides a convenient and efficient physical criterion to discriminate the stages of the spinodal decomposition and domain growth. Via the DBM simulation and this criterion, we quantitatively study the effects of latent heat and surface tension on phase separation. It is found that the TNE strength attains its maximum at the end of the spinodal decomposition stage, and it decreases when the latent heat increases from zero. The surface tension effects are threefold, prolong the duration of the spinodal decomposition stage, decrease the maximum TNE intensity, and accelerate the speed of the domain growth stage.

Journal ArticleDOI
TL;DR: It is found that the stain gradually changes from the usually observed ring to an "eye" shape, that is, a combination of the thick central stain and the thin outer ring, with potential applications in self-assembly and ink-jet printing.
Abstract: We discuss how the stain left after evaporation of a suspension evolves with heating of the glass or plastic on which the liquid has been deposited. Upon increasing the substrate temperature, it is found that the stain gradually changes from the usually observed ring to an “eye” shape, that is, a combination of the thick central stain and the thin outer ring. Both the size and the relative volume of the central stain increase with the substrate temperature. The main mechanism for this phenomenon is proposed to be an enhanced Marangoni recirculation flow on hot substrates. These findings can be exploited to continuously tune the morphology of coffee stains, with potential applications in self-assembly and ink-jet printing.

Journal ArticleDOI
TL;DR: In this article, the deformation of a particle at an interface is governed by a competition of bulk elasticity and surface tension, which can increase adsorption energies by orders of magnitude relative to rigid particles.
Abstract: Soft particles can be better emulsifiers than hard particles because they stretch at fluid interfaces. This deformation can increase adsorption energies by orders of magnitude relative to rigid particles. The deformation of a particle at an interface is governed by a competition of bulk elasticity and surface tension. When particles are partially wet by the two liquids, deformation is localized within a material-dependent distance L from the contact line. At the contact line, the particle morphology is given by a balance of surface tensions. When the particle radius R≪L, the particle adopts a lenticular shape identical to that of an adsorbed fluid droplet. Particle deformations can be elastic or plastic, depending on the relative values of the Young modulus, E, and yield stress, σp. When surface tensions favour complete spreading of the particles at the interface, plastic deformation can lead to unusual fried-egg morphologies. When deformable particles have surface properties that are very similar to one liquid phase, adsorption can be extremely sensitive to small changes of their affinity for the other liquid phase. These findings have implications for the adsorption of microgel particles at fluid interfaces and the performance of stimuli-responsive Pickering emulsions.

Journal ArticleDOI
TL;DR: The objective of this paper is to summarize and evaluate scientific advances in clay mineral-containing nanocomposite hydrogels in terms of their specific preparation, formation mechanisms, properties, and applications, and to identify the prevailing challenges and future directions in the field.
Abstract: Clay mineral-containing nanocomposite hydrogels have been proven to have exceptional composition, properties, and applications, and consequently have attracted a significant amount of research effort over the past few years. The objective of this paper is to summarize and evaluate scientific advances in clay mineral-containing nanocomposite hydrogels in terms of their specific preparation, formation mechanisms, properties, and applications, and to identify the prevailing challenges and future directions in the field. The state-of-the-art of existing technologies and insights into the exfoliation of layered clay minerals, in particular montmorillonite and LAPONITE®, are discussed first. The formation and structural characteristics of polymer/clay nanocomposite hydrogels made from in situ free radical polymerization, supramolecular assembly, and freezing-thawing cycles are then examined. Studies indicate that additional hydrogen bonding, electrostatic interactions, coordination bonds, hydrophobic interaction, and even covalent bonds could occur between the clay mineral nanoplatelets and polymer chains, thereby leading to the formation of unique three-dimensional networks. Accordingly, the hydrogels exhibit exceptional optical and mechanical properties, swelling-deswelling behavior, and stimuli-responsiveness, reflecting the remarkable effects of clay minerals. With the pivotal roles of clay minerals in clay mineral-containing nanocomposite hydrogels, the nanocomposite hydrogels possess great potential as superabsorbents, drug vehicles, tissue scaffolds, wound dressing, and biosensors. Future studies should lay emphasis on the formation mechanisms with in-depth insights into interfacial interactions, the tactical functionalization of clay minerals and polymers for desired properties, and expanding of their applications.

Journal ArticleDOI
TL;DR: This study uses giant unilamellar vesicles (GUVs) to measure passive transport across membranes containing defined concentrations of oxidized lipid species, finding the relationship between oxidation and permeation could provide insight into the pharmaceutical characteristics of tissues with oxidative damage.
Abstract: Oxidation of unsaturated lipids in cellular membranes has been shown to cause severe membrane damage and potentially cell death. The presence of oxidized lipid species in the membrane is known to cause changes in membrane properties, such as decreased fluidity. This study uses giant unilamellar vesicles (GUVs) to measure passive transport across membranes containing defined concentrations of oxidized lipid species. GUVs consisting of a saturated phospholipid, an unsaturated phospholipid, and cholesterol were used as model membranes. By replacing defined amounts of the unsaturated lipid with a corresponding oxidized product, the oxidation process could be mimicked, yielding vesicles of varying oxidized lipid concentration. Oxidized lipid concentration was varied from 0 mol% to 18 mol% of the total lipid concentration. Passive transport of PEG12-NBD, an uncharged fluorescent molecule, was measured using a microfluidic trap to capture the GUVs and spinning disk confocal microscopy (SDCM) to track the transport of a fluorescent species in the equatorial plane of each GUV. Membrane permeability was determined by fitting the resulting concentration profiles to a finite difference model of diffusion and permeation around and through the membrane. Experiments showed three permeability regimes. Without oxidation, transport was slow, with a measured permeability on the order of 1.5 × 10−6 cm s−1. At 2.5–10% oxidized species permeation was fast (1.5 × 10−5 cm s−1). Above 12.5% oxidized species, the bilayer was disrupted by the formation of pore defects. As passive transport is an important mechanism for drug delivery, understanding the relationship between oxidation and permeation could provide insight into the pharmaceutical characteristics of tissues with oxidative damage.

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TL;DR: Four typical aspects of femtosecond laser induced special wettable: superhydrophobicity, underwater superoleophobicity, anisotropic wettability, and smart wettabilities are introduced.
Abstract: Femtosecond laser microfabrication is emerging as a hot tool for controlling the wettability of solid surfaces. This paper introduces four typical aspects of femtosecond laser induced special wettability: superhydrophobicity, underwater superoleophobicity, anisotropic wettability, and smart wettability. The static properties are characterized by the contact angle measurement, while the dynamic features are investigated by the sliding behavior of a liquid droplet. Using different materials and machining methods results in different rough microstructures, patterns, and even chemistry on the solid substrates. So, various beautiful wettabilities can be realized because wettability is mainly dependent on the surface topography and chemical composition. The distinctions of the underlying formation mechanism of these wettabilities are also described in detail.

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TL;DR: It is shown that the choice and amount of organic solvent allows the rheological properties of the gel to be tuned, and the differences in properties arise from the microstructure of the fibre network formed.
Abstract: Gels can be formed by dissolving Fmoc–diphenylalanine (Fmoc–PhePhe or FmocFF) in an organic solvent and adding water. We show here that the choice and amount of organic solvent allows the rheological properties of the gel to be tuned. The differences in properties arise from the microstructure of the fibre network formed. The organic solvent can then be removed post-gelation, without significant changes in the rheological properties. Gels formed using acetone are meta-stable and crystals of FmocFF suitable for X-ray diffraction can be collected from this gel.

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TL;DR: This article focuses, in particular, on selected examples of unprecedented topology effects of cyclic polymers upon self-assemblies, dynamics and responses, to highlight current progress in Topological Polymer Chemistry.
Abstract: A variety of single- and multicyclic polymers having programmed chemical structures with guaranteed purity have now become obtainable owing to a number of synthetic breakthroughs achieved in recent years. Accordingly, a broadening range of studies has been undertaken to gain updated insights on fundamental polymer properties of cyclic polymers in either solution or bulk, in either static or dynamic states, and in self-assemblies, leading to unusual properties and functions of polymer materials based on their cyclic topologies. In this article, we review recent studies aiming to achieve distinctive properties and functions by cyclic polymers unattainable by their linear or branched counterparts. We focus, in particular, on selected examples of unprecedented topology effects of cyclic polymers upon self-assemblies, dynamics and responses, to highlight current progress in Topological Polymer Chemistry.

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TL;DR: It is shown that, for a broad class of spherical active particles, rheotactic behavior may emerge via a mechanism which involves "self-trapping" near a hard wall owing to the active propulsion of the particles, combined with their rotation, alignment, and "locking" of the direction of motion into the shear plane.
Abstract: For active particles the interplay between the self-generated hydrodynamic flow and an external shear flow, especially near bounding surfaces, can result in a rich behavior of the particles not easily foreseen from the consideration of the active and external driving mechanisms in isolation. For instance, under certain conditions, the particles exhibit “rheotaxis”, i.e., they align their direction of motion with the plane of shear spanned by the direction of the flow and the normal of the bounding surface and move with or against the flow. To date, studies of rheotaxis have focused on elongated particles (e.g., spermatozoa), for which rheotaxis can be understood intuitively in terms of a “weather vane” mechanism. Here we investigate the possibility that spherical active particles, for which the “weather vane” mechanism is excluded due to the symmetry of the shape, may nevertheless exhibit rheotaxis. Combining analytical and numerical calculations, we show that, for a broad class of spherical active particles, rheotactic behavior may emerge via a mechanism which involves “self-trapping” near a hard wall owing to the active propulsion of the particles, combined with their rotation, alignment, and “locking” of the direction of motion into the shear plane. In this state, the particles move solely up- or downstream at a steady height and orientation.