Suvendu Mandal

Multiple reentrant glass transitions in confined hard-sphere glasses

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.

Shear-induced anisotropic decay of correlations in hard-sphere colloidal glasses

Spatial correlations of microscopic fluctuations are investigated via real-space experiments and computer simulations of colloidal glasses under steady shear. It is shown that while the distribution of one-particle fluctuations is always isotropic regardless of the relative importance of shear as compared to thermal fluctuations, their spatial correlations show a marked sensitivity to the competition between shear-induced and thermally activated relaxation. Correlations are isotropic in the thermally dominated regime, but develop strong anisotropy as shear dominates the dynamics of microscopic fluctuations. We discuss the relevance of this observation for a better understanding of flow heterogeneity in sheared amorphous solids.

Correlations of plasticity in sheared glasses

In a recent paper [Mandal et al., Phys. Rev. E 88, 022129 (2013)], the nature of spatial correlations of plasticity in hard-sphere glasses was addressed both via computer simulations and in experiments. It was found that the experimentally obtained correlations obey a power law, whereas the correlations from simulations are better fitted by an exponential decay. We here provide direct evidence-via simulations of a hard-sphere glass in two dimensions (2D)-that this discrepancy is a consequence of the finite system size in the 3D simulations. By extending the study to a 2D soft disk model at zero temperature [Durian, Phys. Rev. Lett. 75, 4780 (1995)], the robustness of the power-law decay in sheared amorphous solids is underlined. Deviations from a power law occur when either reducing the packing fraction towards the supercooled regime in the case of hard spheres or changing the dissipation mechanism from contact dissipation to a mean-field-type drag in the case of soft disks.

Heterogeneous Shear in Hard Sphere Glasses

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.

Single-particle fluctuations and directional correlations in driven hard-sphere glasses

Via event-driven molecular dynamics simulations and experiments, we study the packing-fraction and shear-rate dependence of single-particle fluctuations and dynamic correlations in hard-sphere glasses under shear. At packing fractions above the glass transition, correlations increase as shear rate decreases: the exponential tail in the distribution of single-particle jumps broadens and dynamic four-point correlations increase. Interestingly, however, upon decreasing the packing fraction, a broadening of the exponential tail is also observed, while dynamic heterogeneity is shown to decrease. An explanation for this behavior is proposed in terms of a competition between shear and thermal fluctuations. Building upon our previous studies [Chikkadi et al., Europhys. Lett. 100, 56001 (2012)], we further address the issue of anisotropy of the dynamic correlations.

Diverging Time Scale in the Dimensional Crossover for Liquids in Strong Confinement

We study a strongly interacting dense hard-sphere system confined between two parallel plates by event-driven molecular dynamics simulations to address the fundamental question of the nature of the 3D to 2D crossover. As the fluid becomes more and more confined the dynamics of the transverse and lateral degrees of freedom decouple, which is accompanied by a diverging time scale separating 2D from 3D behavior. Relying on the time-correlation function of the transversal kinetic energy, the scaling behavior and its density dependence is explored. Surprisingly, our simulations reveal that its time dependence becomes purely exponential such that memory effects can be ignored. We rationalize our findings quantitatively in terms of an analytic theory which becomes exact in the limit of strong confinement.

Flow heterogeneity and correlations in a sheared hard sphere glass: Insight from computer simulations

Understanding the origin of flow heterogeneity in glassy systems is of high interest both due to its importance from theoretical standpoint as well as due to its occurrence in a large number of practical situations such as the flow of the so-called soft-glassy materials (foams, colloidal suspensions, granular media, etc). Detailed experimental investigations do indeed confirm that the flow of driven amorphous solids is not homogeneous, even if the macroscopic stress is constant across the system. We study this issue via large scale event driven molecular dynamics simulations of a hard sphere glass. We observe significant fluctuations of the velocity profile with a time scale of the order of a few hundreds percent strain. Furthermore, there appears to be a correlation between the fluctuations of the local volume fraction and the fluctuations of the local shear rate. The time scales of the fluctuations of density and shear rate are practically identical. These observations motivate an interpretation of our ...

Flow and Rheological Response of Model Glasses

Results of molecular dynamics simulations on the response of glassy materials to an externally imposed steady shear are presented. The work highlights on one hand how the competition of the time scale imposed by the flow and the inherent structural relaxation time determines the linear or non-linear nature of the rheological response. On the other hand, the issue of flow heterogeneity in a shear melted glass is also studied.