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Register a new userMultiple reentrant glass transitions in confined hard-sphere glasses
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Glass forming liquids exhibit a rich phenomenology upon confinement. This is often related to the effects arising from wall-fluid interactions. Here we focus on the interesting limit where the separation of the confining walls becomes of the order of a few particle diameters. For a moderately polydisperse, densely packed hard-sphere fluid confined between two smooth hard walls, we show via event-driven molecular dynamics simulations the emergence of a multiple reentrant glass transition scenario upon a variation of the wall separation. Using thermodynamic relations, this reentrant phenomenon is shown to persist also under constant chemical potential. This allows straightforward experimental investigation and opens the way to a variety of applications in micro- and nanotechnology, where channel dimensions are comparable to the size of the contained particles. The results are in-line with theoretical predictions obtained by a combination of density functional theory and the mode-coupling theory of the glass transition.
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There is growing evidence that the flow of driven amorphous solids is not homogeneous, even if the macroscopic stress is constant across the system. Via event driven molecular dynamics simulations of a hard sphere glass, we provide the first direct evidence for a correlation between the fluctuations of the local volume-fraction and the fluctuations of the local shear rate. Higher shear rates do preferentially occur at regions of lower density and vice versa. The temporal behavior of fluctuations is governed by a characteristic time scale, which, when measured in units of strain, is independent of shear rate in the investigated range. Interestingly, the correlation volume is also roughly constant for the same range of shear rates. A possible connection between these two observations is discussed.
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.
We report results of dynamic light scattering measurements of the coherent intermediate scattering function (ISF) of glasses of hard spheres for several volume fractions and a range of scattering vectors around the primary maximum of the static structure factor. The ISF shows a clear crossover from an initial fast decay to a slower non-stationary decay. Ageing is quantified in several different ways. However, regardless of the method chosen, the perfect aged glass is approached in a power-law fashion. In particular, the coupling between the fast and slow decays, as measured by the degree of stretching of the ISF at the crossover, also decreases algebraically with waiting time. The non-stationarity of this coupling implies that even the fastest detectable processes are themselves non-stationary.
We study the flow of concentrated hard-sphere colloidal suspensions along smooth, non-stick walls using cone-plate rheometry and simultaneous confocal microscopy. In the glass regime, the global flow shows a transition from Herschel-Bulkley behavior at large shear rate to a characteristic Bingham slip response at small rates, absent for ergodic colloidal fluids. Imaging reveals both the `solid microstructure during full slip and the local nature of the `slip to shear transition. Both the local and global flow are described by a phenomenological model, and the associated Bingham slip parameters exhibit characteristic scaling with size and concentration of the hard spheres.
The yielding behaviour of hard sphere glasses under large amplitude oscillatory shear has been studied by probing the interplay of Brownian motion and shear-induced diffusion at varying oscillation frequencies. Stress, structure and dynamics are followed by experimental rheology and Browian Dynamics simulations. Brownian motion assisted cage escape dominates at low frequencies while escape through shear-induced collisions at high ones, both related with a yielding peak in $G^{prime prime}$. At intermediate frequencies a novel, for HS glasses, double peak in $G^{prime prime}$ is revealed reflecting both mechanisms. At high frequencies and strain amplitudes a persistent structural anisotropy causes a stress drop within the cycle after strain reversal, while higher stress harmonics are minimized at certain strain amplitudes indicating an apparent harmonic response.
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