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Formation of Laves Phases in Repulsive and Attractive Hard Sphere Suspensions

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 Added by Thomas Palberg
 Publication date 2017
  fields Physics
and research's language is English




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Colloidal Laves phases (LPs) of $MgCu_2$ type are promising precursors for diamond structure photonic materials. They have been predicted for hard sphere binary mixtures, but not yet observed. We here report a time resolved static light scattering study on their formation in a binary mixture of buoyant experimental hard sphere approximants (size ratio $Gamma=0.77$, molar fraction of small spheres $x_S = 0.76$) for volume fractions between melting and the glass transition. In line with theoretical expectation, all samples form LPs of $MgZn_2$ structure on the time scale of weeks to months. $MgNi_2$ structures are absent, $MgCu_2$ structures and randomly stacked LPs prevail at elevated volume fraction. The addition of small amounts of non-adsorbing polymer switches the interaction to depletion attractive and results in significantly accelerated crystallization kinetics and improved crystal quality.



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Discontinuous shear thickening (DST) observed in many dense athermal suspensions has proven difficult to understand and to reproduce by numerical simulation. By introducing a numerical scheme including both relevant hydrodynamic interactions and granularlike contacts, we show that contact friction is essential for having DST. Above a critical volume fraction, we observe the existence of two states: a low viscosity, contactless (hence, frictionless) state, and a high viscosity frictional shear jammed state. These two states are separated by a critical shear stress, associated with a critical shear rate where DST occurs. The shear jammed state is reminiscent of the jamming phase of granular matter. Continuous shear thickening is seen as a lower volume fraction vestige of the jamming transition.
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Diffusion in bidisperse Brownian hard-sphere suspensions is studied by Stokesian Dynamics (SD) computer simulations and a semi-analytical theoretical scheme for colloidal short-time dynamics, based on Beenakker and Mazurs method [Physica 120A, 388 (1983) & 126A, 349 (1984)]. Two species of hard spheres are suspended in an overdamped viscous solvent that mediates the salient hydrodynamic interactions among all particles. In a comprehensive parameter scan that covers various packing fractions and suspension compositions, we employ numerically accurate SD simulations to compute the initial diffusive relaxation of density modulations at the Brownian time scale, quantified by the partial hydrodynamic functions. A revised version of Beenakker and Mazurs $deltagamma$-scheme for monodisperse suspensions is found to exhibit surprisingly good accuracy, when simple rescaling laws are invoked in its application to mixtures. The so-modified $deltagamma$ scheme predicts hydrodynamic functions in very good agreement with our SD simulation results, for all densities from the very dilute limit up to packing fractions as high as $40%$.
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