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Register a new userArrest of flow and emergence of activated processes at the glass transition of a suspension of particles with hard sphere-like interactions
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By combining aspects of the coherent and self intermediate scattering functions, measured by dynamical light scattering on a suspension of hard sphere-like particles, we show that the arrest of particle number density fluctuations spreads from the position of the main structure factor peak. Taking the velocity auto-correlation function into account we propose that as density fluctuations are arrested the systems ability to respond to diffusing momentum currents is impaired and, accordingly, the viscosity increases. From the stretching of the coherent intermediate scattering function we read a quantitative manifestation of the undissipated thermal energy, the source of those, ergodicity restoring, processes that short-circuit the sharp transition to a perfect glass.
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We analyse the experimental particle current auto correlation function (CAF) of suspensions of hard spheres. Interactions between the particles are mediated by thermally activated acoustic excitations in the solvent. Those acoustic modes are tantamount to the systems (energy) microstates and by their orthogonality, each of those modes can be identified with an independent Brownian particle current. Accordingly, partitioning of the systems energy states is impressed on the CAF. This impression provides a novel measure of the entropy and location of a partitioning/entropy limit at a packing fraction that coincides with that of the observed suspensions first order freezing transition.
The complex behavior of confined fluids arising due to a competition between layering and local packing can be disentangled by considering quasi-confined liquids, where periodic boundary conditions along the confining direction restore translational invariance. This system provides a means to investigate the interplay of the relevant length scales of the confinement and the local order. We provide a mode-coupling theory of the glass transition (MCT) for quasi-confined liquids and elaborate an efficient method for the numerical implementation. The nonergodicity parameters in MCT are compared to computer-simulation results for a hard-sphere fluid. We evaluate the nonequilibrium-state diagram and investigate the collective intermediate scattering function. For both methods, nonmonotonic behavior depending on the confinement length is observed.
Colloidal systems observed in video microscopy are often analysed using the displacements correlation matrix of particle positions. In non-thermal systems, the inverse of this matrix can be interpreted as a pair-interaction potential between particles. If the system is thermally agitated, however, only an effective interaction is accessible from the correlation matrix. We show how this effective interaction differs from the non-thermal case by comparing with high-statistics numerical data from hard-sphere crystals.
The solid-solid coexistence of a polydisperse hard sphere system is studied by using the Monte Carlo simulation. The results show that for large enough polydispersity the solid-solid coexistence state is more stable than the single-phase solid. The two coexisting solids have different composition distributions but the same crystal structure. Moreover, there is evidence that the solid-solid transition terminates in a critical point as in the case of the fluid-fluid transition.
The collective dynamics of liquid Gallium close to the melting point has been studied using Inelastic X-ray Scattering to probe lengthscales smaller than the size of the first coordination shell. %(momentum transfers, $Q$, $>$15 nm$^{-1}$). Although the structural properties of this partially covalent liquid strongly deviate from a simple hard-sphere model, the dynamics, as reflected in the quasi-elastic scattering, are beautifully described within the framework of the extended heat mode approximation of Enskogs kinetic theory, analytically derived for a hard spheres system. The present work demonstrates the applicability of Enskogs theory to non hard- sphere and non simple liquids.
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