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J Bergenholtz

Publications and source records attributed to J Bergenholtz.

6 recordsLinked to original sources

Small-angle neutron scattering on a core-shell colloidal system: a contrast-variation study.

Small-angle neutron scattering (SANS) measurements are reported on a sterically stabilized, core-shell colloidal system using contrast variation. Aqueous dispersions of polystyrene particles bearing grafted poly(ethylene glycol) (PEG) have been studied over a large range of particle concentrations and two different solvent conditions for the PEG polymer. SANS data are analyzed quantitatively by modeling the particles as core-shell colloids. In a good solvent and under particle contrast conditions, an effective hard-sphere interaction captures excluded-volume interactions up to high concentrations. Contrast variation, through isotopic substitution of both the core and solvent, expedite a detailed study of the PEG layer, both in the dilute limit and as a function of the particle concentration. Upon diminishing the solvent quality, subtle changes in the PEG layer translate into attractions among particles of moderate magnitude.

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Depletion interactions in model microemulsions.

The effects of temperature changes and polymer addition on the behavior of droplet microemulsions of nonionic surfactant, water, and decane are reported and analyzed within polymer depletion theory. Dilution viscometry and dynamic light scattering were used to confirm that these microemulsions behave essentially as hard-sphere dispersions, providing us with an ideal reference system. Addition of poly(ethylene glycol) (PEG) lowers the emulsification failure boundary, where excess oil is expelled, which can be qualitatively understood by an analysis of the available volume for the polymer. Sufficient addition of PEG causes a fluid-fluid phase separation in qualitative accord with experiments on mixtures of rigid colloidal hard spheres and nonadsorbing polymer. Addition of PEG or raising the temperature causes the collective diffusion coefficient D(C) to decrease. From theory, the initial linear slope of D(C) versus droplet concentration can be used to discriminate between attractions and repulsions. The measured D(C) data for the droplets in the presence of PEG are modeled using the Asakura-Oosawa theory of depletion. Fitting the theory to the measured D(C) data permits for extracting the only unknown parameter, the polymer radius of gyration. Quantitative agreement is found with literature data, demonstrating that polymer depletion occurs in the system and that the Asakura-Oosawa theory provides a faithful description of the phenomenon.

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Multiple glassy states in a simple model system.

Experiments, theory, and simulation were used to study glass formation in a simple model system composed of hard spheres with short-range attraction ("sticky hard spheres"). The experiments, using well-characterized colloids, revealed a reentrant glass transition line. Mode-coupling theory calculations and molecular dynamics simulations suggest that the reentrance is due to the existence of two qualitatively different glassy states: one dominated by repulsion (with structural arrest due to caging) and the other by attraction (with structural arrest due to bonding). This picture is consistent with a study of the particle dynamics in the colloid using dynamic light scattering.

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Hydrodynamic and Colloidal Interactions in Concentrated Charge-Stabilized Polymer Dispersions.

Hydrodynamic and colloidal interactions are explored in concentrated, charge-stabilized colloidal dispersions by measuring the dependence of rheology (e.g., low and high-shear viscosity, high-frequency viscosity, and modulus) and self-diffusivity on salt content, particle size, and concentration. Model, sulfonated polystyrene lactices of varying diameter are prepared and investigated by shear rheology, high-frequency torsional resonance, electrophoresis, titration, and dynamic light scattering. The high-frequency and high-shear viscosity both are dominated by hydrodynamic interactions, but are shown not to be identical, due to the microstructure distortion resulting from high shear rates. The short-time self-diffusion is also shown to be insensitive to direct particle interactions, but has a different concentration dependence than the high-frequency viscosity, further illustrating a predicted violation of a generalized Stokes-Einstein relationship for these properties. The apparent colloidal surface charge is extracted from the high-frequency elastic modulus measurements on concentrated dispersions. The surface charge is in good agreement with results from critical coagulation concentration measurements and perturbation theories, but disagrees with electrophoretic mobility experiments. This indicates that the effective surface charge determined by torsional high-frequency measurements is a more reliable predicter of the salt stability of charge-stabilized dispersions, in comparison to zeta-potentials determined from electrophoretic mobilities. Further, we demonstrate by direct comparison that measurements of the apparent plateau modulus by rotational rheometry underestimate the true, high-frequency modulus and provide unreliable estimates for the surface charge. Copyright 2000 Academic Press.

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Nonergodicity transitions in colloidal suspensions with attractive interactions.

Colloidal gel and glass transitions are investigated using the idealized mode coupling theory (MCT) for model systems characterized by short-range attractive interactions. Results are presented for adhesive hard sphere and hard core attractive Yukawa systems. According to MCT, the former system shows a critical glass transition concentration that increases significantly with introduction of a weak attraction. For the latter attractive Yukawa system, MCT predicts low temperature nonergodic states that extend to the critical and subcritical region. Several features of the MCT nonergodicity transition in this system agree qualitatively with experimental observations on the colloidal gel transition, suggesting that the gel transition is caused by a low temperature extension of the glass transition. The range of the attraction is shown to govern the way the glass transition line traverses the phase diagram relative to the critical point, analogous to findings for the fluid-solid freezing transition.

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