To describe the full spectrum of surface fluctuations of the interface between phase-separated colloid-polymer mixtures from low scattering vector q (classical capillary wave theory) to high q (bulk-like fluctuations), one must take account of the interface's bending rigidity. We find that the bending rigidity is negative and that on approach to the critical point it vanishes proportionally to the interfacial tension. Both features are in agreement with Monte Carlo simulations.
Colloidal suspensions with free polymer coils which are larger than the colloidal particles are considered. The polymer-colloid interaction is modeled by an extension of the Asakura-Oosawa model. Phase separation occurs into dilute and dense fluid phases of colloidal particles when polymer is added. The critical density of this transition tends to zero as the size of the polymer coils diverges.
We consider a model mixture of hard colloidal spheres and non-adsorbing polymer chains in a theta solvent. The polymer component is modelled as a polydisperse mixture of effective spheres, mutually noninteracting but excluded from the colloids, with radii that are free to adjust to allow for colloid-induced compression. We investigate the bulk fluid demixing behaviour of this model system using a geometry-based density-functional theory that includes the polymer size polydispersity and configurational free energy, obtained from the exact radius-of-gyration distribution for an ideal (random-wal…
Fluctuations of the interface between coexisting colloidal fluid phases have been measured with confocal microscopy. Due to a very low surface tension, the thermal motions of the interface are so slow, that a record can be made of the positions of the interface. The theory of the interfacial height fluctuations is developed. For a host of correlation functions, the experimental data are compared with the theoretical expressions. The agreement between theory and experiment is remarkably good.
The depletion interactions between two colloidal plates or between two colloidal spheres, induced by interacting polymers in a good solvent, are calculated theoretically and by computer simulations. A simple analytical theory is shown to be quantitatively accurate for case of two plates. A related depletion potential is derived for two spheres; it also agrees very well with direct computer simulations. Theories based on ideal polymers show important deviations with increasing polymer concentration: They overestimate the range of the depletion potential between two plates or two spheres at all …
We investigate the structure of colloid-polymer mixtures by calculating the structure factors for the Asakura-Oosawa model in the PY approximation. We discuss the role of potential range, polymer concentration and polymer-polymer interactions on the colloid-colloid structure. Our results compare reasonably well with the recent experiments of Moussaïd et. al. for small wavenumber $k$, but we find that the Hansen-Verlet freezing criterion is violated when the liquid phase becomes marginal.
We consider a ternary mixture of hard colloidal spheres, ideal polymer spheres, and rigid vanishingly thin needles, which model stretched polymers or colloidal rods. For this model we develop a geometry-based density functional theory, apply it to bulk fluid phases, and predict demixing phase behavior. In the case of no polymer-needle interactions, two-phase coexistence between colloid-rich and -poor phases is found. For hard needle-polymer interactions we predict rich phase diagrams, exhibiting three-phase coexistence, and reentrant demixing behavior.
We show how to coarse grain polymers in a good solvent as single particles, interacting with density-independent or density-dependent interactions. These interactions can be between the centres of mass, the mid-points or end-points of the polymers. We also show how to extend these methods to polymers in poor solvents and mixtures of polymers. Treating polymers as soft colloids can greatly speed up the simulation of complex many-polymer systems, including polymer-colloid mixtures.
Surface effects are generally prevailing in confined colloidal systems. Here we report on dispersed nanoparticles close to a fluid membrane. Exact results regarding the static organization are derived for a dilute solution of non-adhesive colloids. It is shown that thermal fluctuations of the membrane broaden the density profile, but on average colloids are neither accumulated nor depleted near the surface. The radial correlation function is also evaluated, from which we obtain the effective pair-potential between colloids. This entropically-driven interaction shares many similarities with the…
We study theoretically the equilibrium phase behaviour of a mixture of polydisperse hard-sphere colloids and monodisperse polymers, modelled using the Asakura-Oosawa model within the free volume approximation of Lekkerkerker et al. We compute full phase diagrams in the plane of colloid and polymer volume fractions, using the moment free energy method. The intricate features of phase separation in pure polydisperse colloids combine with the appearance of polymer-induced gas-liquid coexistence to give a rich variety of phase diagram topologies as the polymer-colloid size ratio and the colloid po…
We study the structure and interfacial properties of model athermal mixtures of colloids and excluded volume polymers. The colloid particles are modeled as hard spheres whereas the polymer coils are modeled as chains formed from tangentially bonded hard spheres. Within the framework of the nonlocal density functional theory we study the influence of the chain length on the surface tension and the interfacial width. We find that the interfacial tension of the colloid-interacting polymer mixtures increases with the chain length and is significantly smaller than that of the ideal polymers. For ce…
We investigate the response to temperature of a well-known colloid-polymer mixture. At room temperature, the critical value of the second virial coefficient of the effective interaction for the Asakura-Oosawa model predicts the onset of gelation with remarkable accuracy. Upon cooling the system, the effective attractions between colloids induced by polymer depletion are reduced, because the polymer radius of gyration is decreases as the theta-temperature is approached. Paradoxically, this raises the effective temperature, leading to "melting" of colloidal gels. We find the Asakura-Oosawa model…
Interfacial properties of colloid--polymer mixtures are examined within an effective one--component representation, where the polymer degrees of freedom are traced out, leaving a fluid of colloidal particles interacting via polymer--induced depletion forces. Restriction is made to zero, one and two--body effective potentials, and a free energy functional is used which treats colloid excluded volume correlations within Rosenfeld's Fundamental Measure Theory, and depletion--induced attraction within first--order perturbation theory. This functional allows a consistent treatment of both ideal and…
As first explained by the classic Asakura-Oosawa (AO) model, effective attractive forces between colloidal particles induced by depletion of nonadsorbing polymers can drive demixing of colloid-polymer mixtures into colloid-rich and colloid-poor phases, with practical relevance for purification of water, stability of foods and pharmaceuticals, and macromolecular crowding in biological cells. By idealizing polymer coils as effective penetrable spheres, the AO model qualitatively captures the influence of polymer depletion on thermodynamic phase behavior of colloidal suspensions. In previous work…
We report a numerical study of equilibrium phase-diagrams and interfacial properties of bulk and confined colloid-polymer mixtures using grand canonical Monte Carlo simulations. Colloidal particles are treated as hard spheres, while the polymer chains are described as soft repulsive spheres. The polymer-polymer, colloid-polymer, and wall-polymer interactions are described by density-dependent potentials derived by Bolhuis and Louis [Macromolecules, 35 (2002), p.1860]. We compared our results with those of the Asakura-Oosawa-Vrij model, that treats the polymers as ideal particles. We find that …
We present a theoretical approach which maps polymer blends onto mixtures of soft-colloidal particles. The analytical mesoscale pair distribution functions reproduce well data from united atom molecular dynamics simulations of polyolefin mixtures without fitting parameters. The theory exactly recovers the analytical expressions for density and concentration fluctuation structure factors of soft colloidal mixtures (liquid alloys).
The change of the structure of concentrated colloidal suspensions upon addition of non-adsorbing polymer is studied within a two-component, Ornstein-Zernicke based liquid state approach. The polymers' conformational degrees of freedom are considered and excluded volume is enforced at the segment level. The polymer correlation hole, depletion layer, and excess chemical potentials are described in agreement with polymer physics theory in contrast to models treating the macromolecules as effective spheres. Known depletion attraction effects are recovered for low particle density, while at higher …
We study the depletion-induced self-assembly of indented colloids. Using state-of-the-art Monte Carlo simulation techniques that treat the depletant particles explicitly, we demonstrate that colloids assemble by a lock-and-key mechanism, leading to colloidal polymerization. The morphology of the chains that are formed depends sensitively on the size of the colloidal indentation, with smaller values additionally permitting chain branching. In contrast to the case of spheres with attractive patches, Wertheim's thermodynamic perturbation theory fails to provide a fully quantitative description of…
We consider a binary mixture of colloid and polymer particles with positions on a simple cubic lattice. Colloids exclude both colloids and polymers from nearest neighbor sites. Polymers are treated as effective particles that are mutually non-interacting, but exclude colloids from neighboring sites; this is a discrete version of the (continuum) Asakura-Oosawa-Vrij model. Two alternative density functionals are proposed and compared in detail. The first is based on multi-occupancy in the zero-dimensional limit of the bare model, analogous to the corresponding continuum theory that reproduces th…
Theory and simulation of Brownian colloids suspended in an implicit solvent, with the hydrodynamics of the fluid accounted for by effective interactions between the colloids, are shown to yield a marked and hitherto unobserved discrepancy between the viscosity calculated from the average shear stress under an imposed shear rate in the Stokesian regime and the viscosity extracted by the Green-Kubo formalism from the auto-correlations of thermal stress fluctuations in quiescent equilibrium. We show that agreement between both methods is recovered by accounting for the fluctuating Brownian stress…
The surface tension of interacting polymers in a good solvent is calculated theoretically and by computer simulations for a planar wall geometry and for the insertion of a single colloidal hard-sphere. This is achieved for the planar wall and for the larger spheres by an adsorption method, and for smaller spheres by a direct insertion technique. Results for the dilute and semi-dilute regimes are compared to results for ideal polymers, the Asakura-Oosawa penetrable-sphere model, and to integral equations, scaling and renormalization group theories. The largest relative changes with density are …
We use a microscopic density functional theory based on Wertheim's first order thermodynamic perturbation theory to study wetting behavior of athermal mixtures of colloids and excluded-volume polymers. In opposition to the wetting behavior of the Asakura-Oosawa-Vrij model we find the polymer-rich phase to wet a hard wall. The wetting transition is of the first order and is accompanied by the prewetting transition. We do not find any hints for the layering transitions in the partial wetting regime. Our results resemble the wetting behavior in athermal polymer solutions. We point out that an acc…
The structural and thermodynamic properties of mixtures of colloidal spheres and non-adsorbing polymer chains are studied within a novel general two-component macromolecular liquid state approach applicable for all size asymmetry ratios. The dilute limits, when one of the components is at infinite dilution but the other concentrated, are presented and compared to field theory and models which replace polymer coils with spheres. Whereas the derived analytical results compare well, qualitatively and quantitatively, with mean-field scaling laws where available, important differences from ``effect…
We map dilute or semi-dilute solutions of non-intersecting polymer chains onto a fluid of ``soft'' particles interacting via a concentration dependent effective pair potential, by inverting the pair distribution function of the centers of mass of the initial polymer chains. A similar inversion is used to derive an effective wall-polymer potential; these potentials are combined to successfully reproduce the calculated exact depletion interaction induced by non-intersecting polymers between two walls. The mapping opens up the possibility of large-scale simulations of polymer solutions in complex…
Depletion-induced interactions between colloids in colloid-polymer mixtures depend in range and strength on size, shape, and concentration of depletants. Crowding by colloids in turn affects shapes of polymer coils, such as biopolymers in biological cells. By simulating hard-sphere colloids and random-walk polymers, modeled as fluctuating ellipsoids, we compute depletion-induced potentials and polymer shape distributions. Comparing results with exact density-functional theory calculations, molecular simulations, and experiments, we show that polymer shape fluctuations play an important role in…
We consider a simplified coarse-grained model for colloid-polymer mixtures, in which polymers are represented as monoatomic molecules interacting by means of pair potentials. We use it to study polymer-colloid segregation in the presence of a quenched matrix of colloidal hard spheres. We fix the polymer-to-colloid size ratio to 0.8 and consider matrices such that the fraction f of the volume that is not accessible to the colloids due to the matrix is equal to 40%. As in the Asakura-Oosawa-Vrij (AOV) case, we find that binodal curves in the polymer and colloid volume-fraction plane have a small…
The density profile and surface tension for the interface of phase-separated colloid-polymer mixtures have been studied in the framework of the square gradient approximation for both ideal and interacting polymers in good solvent. The calculations show that in the presence of polymer-polymer excluded volume interactions the interfaces have lower widths and surface tensions compared to the case of ideal polymers. These results are a direct consequence of the shorter range and smaller depth of the depletion potential between colloidal particles induced by interacting polymers.
Using video-microscopy imaging we demonstrate the existence of a short-ranged equilibrium attraction between heavy silica colloids diffusing on soft surfaces of cross-linked polymer gels. The inter-colloid potential can be tuned by changing the gel stiffness or by coating the colloids with a polymer layer. On sufficiently soft substrates, the interaction induced by the polymer matrix leads to large-scale colloidal aggregation. We correlate the in-plane interaction with a colloid-surface attraction.
We extensively investigated the critical behavior of mixtures of colloids and polymers via the two-component Asakura-Oosawa model and its reduction to a one-component colloidal fluid using accurate theoretical and simulation techniques. In particular the theoretical approach, hierarchical reference theory [Adv. Phys. 44, 211 (1995)], incorporates realistically the effects of long-range fluctuations on phase separation giving exponents which differ strongly from their mean-field values, and are in good agreement with those of the three-dimensional Ising model. Computer simulations combined with…
The influence of poor solvent quality on fluid demixing of a model mixture of colloids and nonadsorbing polymers is investigated using density functional theory. The colloidal particles are modelled as hard spheres and the polymer coils as effective interpenetrating spheres that have hard interactions with the colloids. The solvent is modelled as a two-component mixture of a primary solvent, regarded as a background theta-solvent for the polymer, and a cosolvent of point particles that are excluded from both colloids and polymers. Cosolvent exclusion favors overlap of polymers, mimicking the e…
We investigate with Monte Carlo computer simulations the capillary phase behaviour of model colloid-polymer mixtures confined between a flat wall and a corrugated wall. The corrugation is modelled via a sine wave as a function of one of the in-plane coordinates leading to a depletion attraction between colloids and the corrugated wall that is curvature dependent. We find that for increased amplitude of corrugation the region of the phase diagram where capillary condensation occurs becomes larger. We derive a Kelvin equation for this system and compare its predictions to the simulation results.…
In drying liquid films of polymer-colloid mixtures, the stratification in which polymers are placed on top of larger colloids is studied. It is often presumed that the formation of segregated polymer-colloid layers is solely due to the proportion in size at fast evaporation as in binary colloid mixtures. By comparing experiments with a theoretical model, we found that the transition in viscosity near the drying interface was another important parameter for controlling the formation of stratified layers in polymer-colloid mixtures. At high evaporation rates, increased polymer concentrations nea…
There have been increasing reports that the diffusion coefficient of macromolecules depends on time and fluctuates randomly. Here, a novel method to elucidate the fluctuating diffusivity from trajectory data is developed. The time-averaged mean square displacement (MSD), a common tool in single-particle-tracking (SPT) experiments, is generalized into a second order tensor, with which information on both magnitude fluctuations and orientational fluctuations of the diffusivity can be clearly detected. This new method is utilized to analyze the center-of-mass motion of four polymer models, the Ro…
An extension of the Asakura-Oosawa-Vrij model of hard sphere colloids and non-adsorbing polymers, that takes polymer non-ideality into account through a repulsive stepfunction pair potential between polymers, is studied with grand canonical Monte Carlo simulations and density functional theory. Simulation results validate previous theoretical findings for the shift of the bulk fluid demixing binodal upon increasing strength of polymer-polymer repulsion, promoting the tendency to mix. For increasing strength of the polymer-polymer repulsion, simulation and theory consistently predict the interf…
We determine the depletion-induced phase-behavior of hard sphere colloids and interacting polymers by large-scale Monte Carlo simulations using very accurate coarse-graining techniques. A comparison with standard Asakura-Oosawa model theories and simulations shows that including excluded volume interactions between polymers leads to qualitative differences in the phase diagrams. These effects become increasingly important for larger relative polymer size. Our simulations results agree quantitatively with recent experiments.
Using self-consistent field and density-functional theories, we first investigate colloidal self-assembling of colloid/polymer films confined between two soft surfaces grafted by polymers. With the increase of colloidal concentrations, the film undergoes a series of transitions from disordered liquid $\to$ sparse square $\to$ hexagonal (or mixed square-hexagonal) $\to$ dense square $\to$ cylindric structures in plane, which results from the competition between the entropic elasticity of polymer brushes and the steric packing effect of colloidal particles. A phase diagram displays the stable re…
From microscopic fluid clusters to macroscopic droplets, the structure of fluids is governed by the Van der Waals force, a force that acts between polarizable objects. In this Letter, we derive a general theory that describes the non-equilibrium counterpart to the Van der Waals force, which emerges in spatially coherently fluctuating electromagnetic fields. We describe the formation of a novel and complex hierarchy of self-organized morphologies in magnetic and dielectric colloid systems. Most striking among these morphologies are dipolar foams - colloidal superstructures that swell against gr…
From studies via Molecular Dynamics simulations, we report results on structure and dynamics in mixtures of active colloids and passive polymers that are confined inside a spherical container with a repulsive boundary. Such systems mimic the presence of bacteria in the background of bio-polymers. All interactions in the fully passive case are chosen in such a way that in equilibrium coexistence between colloid-rich and polymer-rich phases occurs. For most part of the studies the chosen compositions give rise to Janus structure; one side of the sphere is occupied by the colloids and the rest by…
We present Monte Carlo simulations of colloidal particles pulled into grafted polymer layers by external fields. The insertion free energy of a single colloid into the polymer layer is qualitatively different for surfaces with an ordered and a disordered distribution of grafting points. Moreover, the tendency of colloidal particles to traverse the grafting layer is strongly size dependent. In dense colloidal suspensions, under the influence of sufficiently strong external force, a collective instability allows the colloids to penetrate and form internally ordered, columnar structures spanning …
We show that the critical behavior of a colloid-polymer mixture inside a random porous matrix of quenched hard spheres belongs to the universality class of the random-field Ising model. We also demonstrate that random-field effects in colloid-polymer mixtures are surprisingly strong. This makes these systems attractive candidates to study random-field behavior experimentally.
We study fluid-fluid phase separation in a colloid-polymer mixture adsorbed in a colloidal porous matrix close to the θ-point. For this purpose we consider the Asakura-Oosawa model in the presence of a quenched matrix of colloidal hard spheres. We study the dependence of the demixing curve on the parameters that characterize the quenched matrix, fixing the polymer-to-colloid size ratio to 0.8. We find that, to a large extent, demixing curves depend only on a single parameter f, which represents the volume fraction which is unavailable to the colloids. We perform Monte Carlo simulations for vol…
We demonstrate a novel route of spatially organizing the colloid arrangements on the polymer-grafted substrate by use of self-consistent field and density functional theories. We find that grafting of polymers onto a substrate can effectively control spatial dispersions of deposited colloids as a result of the balance between colloidal settling force and entropically elastic force of brushes, and colloids can form unexpected ordered structures on a grafting substrate. The depositing process of colloidal particles onto the elastic "soft" substrate includes two steps: brush-mediated one-dimensio…
We use thermodynamic perturbation theory to calculate the free energies and resulting phase diagrams of binary systems of spherical colloidal particles and interacting polymer coils in good solvent within an effective one-component representation of such mixtures, whereby the colloidal particles interact via a polymer-induced depletion potential. MC simulations are used to test the convergence of the high temperature expansion of the free energy. The phase diagrams calculated for several polymer to colloid size ratios differ considerably from the results of similar calculations for mixtures of…
We study the stability of mixtures of highly screened repulsive charged spheres and non-adsorbing ideal polymer chains in a common solvent using free volume theory. The effective interaction between charged colloids in an aqueous salt solution is described by a screened-Coulomb pair potential, which supplements the pure hard-sphere interaction. The ideal polymer chains are treated as spheres that are excluded from the colloids by a hard-core interaction, whereas the interaction between two ideal chains is set to zero. In addition, we investigate the phase behaviour of charged colloid-polymer m…
We computed the phase-separation behavior and effective interactions of colloid-polymer mixtures in the "protein limit", where the polymer radius of gyration is much larger than the colloid radius. For ideal polymers, the critical colloidal packing fraction tends to zero, whereas for interacting polymers in a good solvent the behavior is governed by a universal binodal, implying a constant critical colloid packing fraction. In both systems the depletion interaction is not well described by effective pair potentials but requires the incorporation of many-body contributions.
We report molecular dynamics simulations of a system of repulsive, polymer-tethered colloidal particles. We use an explicit polymer model to explore how the length and the behavior of the polymer (ideal or self-avoiding) affect the ability of the particles to organize into ordered structures when the system is compressed to moderate volume fractions. We find a variety of different phases whose origin can be explained in terms of the configurational entropy of polymers and colloids. Finally, we discuss and compare our results to those obtained for similar systems using simplified coarse-grained…
Large-scale Monte Carlo simulations of a phase-separating colloid-polymer mixture are performed and compared to recent experiments. The approach is based on effective interaction potentials in which the central monomers of self-avoiding polymer chains are used as effective coordinates. By incorporating polymer nonideality together with soft colloid-polymer repulsion, the predicted binodal is in excellent agreement with recent experiments. In addition, the interfacial tension as well as the capillary length are in quantitative agreement with experimental results obtained at a number of points i…
The influence of confinement, due to flat parallel structureless walls, on phase separation in colloid-polymer mixtures, is investigated by means of grand-canonical Monte Carlo simulations. Ultra-thin films, with thicknesses between $D=3-10$ colloid diameters, are studied. The Asakura-Oosawa model [J. Chem. Phys. 22, 1255 (1954)] is used to describe the particle interactions. To simulate efficiently, a ``cluster move'' [J. Chem. Phys. 121, 3253 (2004)] is used in conjunction with successive umbrella sampling [J. Chem. Phys. 120, 10925 (2004)]. These techniques, when combined with finite size s…
Stable colloidal dispersions with evenly distributed particles are important for many technological applications. Due to Brownian motion colloidal particles have constant collisions with each other which often lead to their aggregation driven by the long range van der Waals attraction. As a result the colloidal systems often tend to precipitate. A number of methods have been devised to minimize the effect of long-range van der Waals attraction between colloidal particles or to override the influence of the attraction in order to provide the colloidal stability.In the PhD thesis we investigated…
We develop the scattering formalism to calculate the interaction between colloidal particles trapped at a fluid interface. Since, in addition to the interface, the colloids may also fluctuate in this system, we implement the fluctuation of the boundaries into the scattering formalism and investigate how the interaction between colloids is modified by their fluctuations. This general method can be applied to any number of colloids with various geometries at an interface. We apply the formalism derived in this work to a system of spherical colloids at the interface between two fluid phases. For …
If particles interact according to isotropic pair potentials that favor multiple length scales, in principle a large variety of different complex structures can be achieved by self-assembly. We present, motivate, and discuss a conjecture for the occurrence of non-trivial (i.e., non-triangular) orderings based on newly-introduced enthalpy-like pair potentials, the capability of which we demonstrate for the specific example of colloid-polymer mixtures. Upon examining the phase behavior of two-dimensional colloid-polymer mixtures, which can also be realized in experiments, we observe that non-tri…
This contribution briefly reviews some recent work demonstrating the partial breakdown of the colloidal fluid <--> atomic fluid analogy. The success of liquid state theory for atomic fluids stems in part from the van der Waals picture, where steric interactions dominate the structure, and attractive interactions can be added as a perturbation. For complex fluids described by effective potentials, this picture may break down. In the first example discussed, depletion potentials in non-additive hard-sphere mixtures are shown to be surprisingly complex, leading to fluid structure and fluid-solid …
Colloid-polymer mixtures may undergo either fluid-fluid phase separation or gelation. This depends on the depth of the quench (polymer concentration) and polymer-colloid size ratio. We present a real-space study of dynamics in phase separating colloid-polymer mixtures with medium- to long-range attractions (polymer-colloid size ratio q_R=0.45-0.89, with the aim of understanding the mechanism of gelation as the range of the attraction is changed. In contrast to previous studies of short-range attractive systems, where gelation occurs shortly after crossing the equilibrium phase boundary, we fin…
We discuss structural correlations in mixtures of free polymer and colloidal particles based on a microscopic, 2-component liquid state integral equation theory. Whereas in the case of polymers much smaller than the spherical particles the relevant polymer degree of freedom is the center of mass, for polymers larger than the (nano-) particles conformational rearrangements need to be considered. They have the important consequence that the polymer depletion layer exhibits two widely different length scales, one of the order of the particle radius, the other of the order of the polymer radius or…
The traction on the surface of a spherical active colloid in a thermally fluctuating Stokesian fluid contains passive, active, and Brownian contributions. Here we derive these three parts systematically, by "projecting out" the fluid using the boundary-domain integral representation of slow viscous flow. We find an exact relation between the statistics of the Brownian traction and the thermal forces in the fluid and derive, thereby, fluctuation-dissipation relations for every irreducible tensorial harmonic traction mode. The first two modes give the Brownian force and torque, from which we con…
Understanding the phase behaviour of mixtures continues to pose challenges, even for systems that might be considered "simple". Here we consider a very simple mixture of two colloidal and one non-adsorbing polymer species which can be simplified even further to a size-asymmetrical binary mixture, in which the effective colloid-colloid interactions depend on the polymer concentration. We show that this basic system exhibits surprisingly rich phase behaviour. In particular, we enquire whether such a system features only a liquid-vapor phase separation (as in one-component colloid-polymer mixture…
We study phase separation and transient gelation in a mixture consisting of polydisperse colloids and non-adsorbing polymers, where the ratio of the average size of the polymer to that of the colloid is approximately 0.063. Unlike what has been reported previously for mixtures with somewhat lower colloid polydispersity, the addition of polymers does not expand the fluid-solid coexistence region. Instead, we find a region of fluid-solid coexistence which has an approximately constant width but an unexpected re-entrant shape. We detect the presence of a metastable gas-liquid binodal, which gives…
The non-equilibrium distribution of colloids in a polymer solution under a temperature gradient is studied experimentally. A slight increase of local temperature by a focused laser drives the colloids towards the hot region, resulting in the trapping of the colloids irrespective of their own thermophoretic properties. An amplification of the trapped colloid density with the polymer concentration is measured, and is quantitatively explained by hydrodynamic theory. The origin of the attraction is a migration of colloids driven by a non-uniform polymer distribution sustained by the polymer's ther…
