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P N Pusey

Publications and source records attributed to P N Pusey.

10 recordsLinked to original sources
PubMed2005

Stability of the binary colloidal crystals AB2 and AB13.

Suspensions of binary mixtures of hard-sphere poly-methylmethacrylate colloidal particles were studied at six different size ratios alpha. The main aim was to determine the range of size ratios over which the binary colloidal crystals AB2 and AB13 are stable. Combining these results with those of earlier work, we found stability of AB2 for 0.60 approximately > alpha approximately > 0.425, in good agreement with theoretical predictions by computer simulation and cell model methods. AB13 was observed for 0.62 approximately > alpha approximately > 0.485, the lower limit being significantly smaller than the theoretical prediction of about 0.525. Rough measurements of crystallization rates showed that AB2 tended to crystallize fastest at small size ratios, whereas the opposite was true for AB13. These findings should provide a guide to the optimum conditions for materials applications of these binary colloidal crystals.

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PubMed2004

Glasses in hard spheres with short-range attraction.

We report a detailed experimental study of the structure and dynamics of glassy states in hard spheres with short-range attraction. The system is a suspension of nearly hard-sphere colloidal particles and nonadsorbing linear polymer which induces a depletion attraction between the particles. Observation of crystallization reveals a reentrant glass transition. Static light scattering shows a continuous change in the static structure factors upon increasing attraction. Dynamic light scattering results, which cover 11 orders of magnitude in time, are consistent with the existence of two distinct kinds of glasses, those dominated by interparticle repulsion and caging, and those dominated by attraction. Samples close to the "A3 point" predicted by mode coupling theory for such systems show very slow, logarithmic dynamics.

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PubMed2002

Rearrangements in hard-sphere glasses under oscillatory shear strain.

We investigate particle rearrangements in colloidal glasses subjected to oscillatory shear strain by the technique of light scattering (LS) echo. LS echo directly follows the motion of the particles through peaks (echoes) in the intensity autocorrelation function; the height of the peak measures the reversible motion in the sample. Polydisperse hard-sphere poly-methylmethacrylate particles were used to avoid crystallization under shear. The yielding behavior is monitored through irreversible particle rearrangements at several volume fractions in the glass phase region. At high volume fractions the glasses are found to yield at strains as high as 15% while the irreversible rearrangements have a more gradual onset with strain for low volume fraction glasses. The behavior of high order echoes at long times is related to the effects of shear on the frozen-in fluctuations of the glass.

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PubMed2002

Structural aging of crystals of hard-sphere colloids.

We report a detailed experimental study of the aging of the (initial) random hexagonal close-packed (rhcp) crystals formed in suspensions of hard-sphere colloids near the melting point. By suspending the same colloidal particles in two different mixtures of solvents we are able to tune the strength of the gravitational forces acting on the particles. The crystal structure is deduced from diffraction patterns measured by the light scattering equivalent of powder x-ray crystallography. A spontaneous aging of the structure is observed over long periods of time, consisting of a fraction of pure face-centered cubic (fcc) crystals growing at the expense of the randomly stacked crystallites. The rate of growth of the new crystals is small and consistent with the predictions by Pronk and Frenkel [13]. Gravity is also revealed to affect the crystals and favor fcc order but through a slow gradual rearrangement of the random stacking. An important new observation is that small mechanical perturbations can strongly affect the structure of the colloidal crystals, promoting fcc growth and interfering with the spontaneous aging process. Previous experimental results are also discussed in the light of these new findings.

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PubMed2002

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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PubMed2001

Phase separation in star-polymer-colloid mixtures.

We examine the demixing transition in star-polymer-colloid mixtures for star arm numbers f=2,6,16,32 and different star-polymer-colloid size ratios 0.18< or =q< or =0.50. Theoretically, we solve the thermodynamically self-consistent Rogers-Young integral equations for binary mixtures using three effective pair potentials obtained from direct molecular computer simulations. The numerical results show a spinodal instability. The demixing binodals are approximately calculated and found to be consistent with experimental observations.

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PubMed2001

Real-space imaging of nucleation and growth in colloidal crystallization.

Crystallization of concentrated colloidal suspensions was studied in real space with laser scanning confocal microscopy. Direct imaging in three dimensions allowed identification and observation of both nucleation and growth of crystalline regions, providing an experimental measure of properties of the nucleating crystallites. By following their evolution, we identified critical nuclei, determined nucleation rates, and measured the average surface tension of the crystal-liquid interface. The structure of the nuclei was the same as the bulk solid phase, random hexagonal close-packed, and their average shape was rather nonspherical, with rough rather than faceted surfaces.

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PubMed1999

Multiple scattering suppression in static light scattering by cross-correlation spectroscopy.

Cross-correlation techniques have been used successfully to suppress multiple scattering in dynamic light-scattering experiments on turbid samples. This allows dynamic information to be obtained straightforwardly by processing the remaining single scattering. Here we show that cross-correlation techniques can also be used to suppress multiple scattering in static light-scattering measurements. We use the two-color dynamic light-scattering method and exploit the fact that the amplitude of the time-dependent part of the measured intensity cross-correlation function depends on the ratio of the single-scattered intensity to the total (single + multiple) scattered intensity. The method is illustrated by measurements of the static structure factors of concentrated suspensions of "hard-sphere" colloids. Good agreement is found with those calculated in the Percus-Yevick approximation.

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