Spinodal Decomposition in a Model Colloid-Polymer Mixture in Microgravity

Bailey, Arthur E.; Poon, Wilson; Christianson, Rebecca J.; Schofield, Andrew B.; Gasser, Urs; Prasad, V.; Manley, Suliana; Segre, Phil; Cipelletti, Luca; Meyer, William V.; Doherty, Michael F.; Sankaran, Subramanian; Jankovsky, Amy; Shiley, William; Bowen, James; Eggers, J.; Kurta, C.; Lorik, Tibor; Pusey, P. N.; Weitz, David A.

doi:10.1103/physrevlett.99.205701

Cited by 95 publications

(104 citation statements)

References 26 publications

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“…Crystallization, vitrification and gelation in systems with short-ranged attractive interactions like colloidal particles and proteins are widely studied phenomena [1,2,3,4,5,6,7,8,9]. Crystallization kinetics is especially important for proteins because good crystals are necessary for the determination of their 3D structure.…”

Section: Introductionmentioning

confidence: 99%

Crystallization and gelation in colloidal systems with short-ranged attractive interactions

2008

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We systematically study the relationship between equilibrium and non-equilibrium phase diagrams of a system of short-ranged attractive colloids. Using Monte Carlo and Brownian dynamics simulations we find a window of enhanced crystallization that is limited at high interaction strength by a slowing down of the dynamics and at low interaction strength by the high nucleation barrier. We find that the crystallization is enhanced by the metastable gas-liquid binodal by means of a two-stage crystallization process. First, the formation of a dense liquid is observed and second the crystal nucleates within the dense fluid. In addition, we find at low colloid packing fractions a fluid of clusters, and at higher colloid packing fractions a percolating network due to an arrested gas-liquid phase separation that we identify with gelation. We find that this arrest is due to crystallization at low interaction energy and it is caused by a slowing down of the dynamics at high interaction strength. Likewise, we observe that the clusters which are formed at low colloid packing fractions are crystalline at low interaction energy, but glassy at high interaction energy. The clusters coalesce upon encounter.

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Section: Introductionmentioning

confidence: 99%

Crystallization and gelation in colloidal systems with short-ranged attractive interactions

2008

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“…), spanning the length scale of 1-10 000 droplets, is the most comprehensive to date for colloidal gels, including measurements by neutron 7 and X-ray scattering, 34 light scattering, 35-37 optical microscopy, 14,38,39 and combinations thereof. Low-f regime.…”

Section: à1åà1mentioning

confidence: 99%

“…35,36,39,45 However, there remains some debate as to the origin of the peak. Some authors have proposed that the peak represents a limiting cluster size, above which effective cluster repulsions (possibly due to excluded volume effects) give rise to the observed clustercluster correlations.…”

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confidence: 99%

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Homogeneous percolation versus arrested phase separation in attractively-driven nanoemulsion colloidal gels

et al. 2014

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We elucidate mechanisms for colloidal gelation of attractive nanoemulsions depending on the volume fraction (f) of the colloid. Combining detailed neutron scattering, cryo-transmission electron microscopy and rheological measurements, we demonstrate that gelation proceeds by either of two distinct pathways. For f sufficiently lower than 0.23, gels exhibit homogeneous fractal microstructure, with a broad gel transition resulting from the formation and subsequent percolation of droplet-droplet clusters.In these cases, the gel point measured by rheology corresponds precisely to arrest of the fractal microstructure, and the nonlinear rheology of the gel is characterized by a single yielding process. By contrast, gelation for f sufficiently higher than 0.23 is characterized by an abrupt transition from dispersed droplets to dense clusters with significant long-range correlations well-described by a model for phase separation. The latter phenomenon manifests itself as micron-scale "pores" within the droplet network, and the nonlinear rheology is characterized by a broad yielding transition. Our studies reinforce the similarity of nanoemulsions to solid particulates, and identify important qualitative differences between the microstructure and viscoelastic properties of colloidal gels formed by homogeneous percolation and those formed by phase separation.

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“…In the SI, we demonstrate that the phase sparation is accommodated by a divergence of the structure factor in the low-k regime, as under microgravity. 21 They are more likely to be seen within the protein regime, whereas crystalline, rather than liquid-like, condensed phases tend to form in the colloid regime. 22 Remarkably, the many-body POMF also predicts this behaviour.…”

Section: Model and Theorymentioning

confidence: 99%

A Many-Body Hamiltonian for Nanoparticles Immersed in a Polymer Solution

Woodward

Forsman

2015

Langmuir

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We develop an analytical theory for the many-body potential of mean force (POMF) between N spheres immersed in a continuum chain fluid. The theory is almost exact for a Θ polymer solution in the protein limit (small particles, long polymers), where N-body effects are important. Polydispersity in polymer length according to a Schulz-Flory distribution emerges naturally from our analysis, as does the transition to the monodisperse limit. The analytical expression for the POMF allows for computer simulations employing the complete N-body potential (i.e., without n-body truncation; n < N ). These are compared with simulations of an explicit particle/polymer mixture. We show that the theory produces fluid structure in excellent agreement with the explicit model simulations even when the system is strongly fluctuating, e.g., at or near the spinodal region. We also demonstrate that other commonly used theoretical approaches, such as truncation of the POMF at the pair level or the Asakura Oosawa model, are extremely inaccurate for these systems.

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Spinodal Decomposition in a Model Colloid-Polymer Mixture in Microgravity

Cited by 95 publications

References 26 publications

Crystallization and gelation in colloidal systems with short-ranged attractive interactions

Crystallization and gelation in colloidal systems with short-ranged attractive interactions

Homogeneous percolation versus arrested phase separation in attractively-driven nanoemulsion colloidal gels

A Many-Body Hamiltonian for Nanoparticles Immersed in a Polymer Solution

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