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Register a new userFundamental differences between glassy dynamics in two and three dimensions
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The two-dimensional freezing transition is very different from its three-dimensional counterpart. In contrast, the glass transition is usually assumed to have similar characteristics in two and three dimensions. Using computer simulations we show that glassy dynamics in supercooled two- and three-dimensional fluids are fundamentally different. Specifically, transient localization of particles upon approaching the glass transition is absent in two dimensions, whereas it is very pronounced in three dimensions. Moreover, the temperature dependence of the relaxation time of orientational correlations is decoupled from that of the translational relaxation time in two dimensions but not in three dimensions. Lastly, the relationships between the characteristic size of dynamically heterogeneous regions and the relaxation time are very different in two and three dimensions. These results strongly suggest that the glass transition in two dimensions is different than in three dimensions.
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We study the glassy dynamics taking place in dense assemblies of athermal active particles that are driven solely by a nonequilibrium self-propulsion mechanism. Active forces are modeled as an Ornstein-Uhlenbeck stochastic process, characterized by a persistence time and an effective temperature, and particles interact via a Lennard-Jones potential that yields well-studied glassy behavior in the Brownian limit, obtained as the persistence time vanishes. By increasing the persistence time, the system departs more strongly from thermal equilibrium and we provide a comprehensive numerical analysis of the structure and dynamics of the resulting active fluid. Finite persistence times profoundly affect the static structure of the fluid and give rise to nonequilibrium velocity correlations that are absent in thermal systems. Despite these nonequilibrium features, for any value of the persistence time we observe a nonequilibrium glass transition as the effective temperature is decreased. Surprisingly, increasing departure from thermal equilibrium is found to promote (rather than suppress) the glassy dynamics. Overall, our results suggest that with increasing persistence time, microscopic properties of the active fluid change quantitatively, but the broad features of the nonequilibrium glassy dynamics observed with decreasing the effective temperature remain qualitatively similar to those of thermal glass-formers.
The question about the existence of a structural glass transition in two dimensions is studied using mode coupling theory (MCT). We determine the explicit d-dependence of the memory functional of mode coupling for one-component systems. Applied to two dimensions we solve the MCT equations numerically for monodisperse hard discs. A dynamic glass transition is found at a critical packing fraction phi_c^{d=2} = 0.697 which is above phi_c^{d=3} = 0.516 by about 35%. phi^d_c scales approximately with phi^d_{rm rcp} the value for random close packing, at least for d=2, 3. Quantities characterizing the local, cooperative cage motion do not differ much for d=2 and d=3, and we e.g. find the Lindemann criterion for the localization length at the glass transition. The final relaxation obeys the superposition principle, collapsing remarkably well onto a Kohlrausch law. The d=2 MCT results are in qualitative agreement with existing results from MC and MD simulations. The mean squared displacements measured experimentally for a quasi-two-dimensional binary system of dipolar hard spheres can be described satisfactorily by MCT for monodisperse hard discs over four decades in time provided the experimental control parameter Gamma (which measures the strength of dipolar interactions) and the packing fraction phi are properly related to each other.
Using overdamped Brownian dynamics simulations we investigate the isotropic-nematic (IN) transition of self-propelled rods in three spatial dimensions. For two well-known model systems (Gay-Berne potential and hard spherocylinders) we find that turning on activity moves to higher densities the phase boundary separating an isotropic phase from a (nonpolar) nematic phase. This active IN phase boundary is distinct from the boundary between isotropic and polar-cluster states previously reported in two-dimensional simulation studies and, unlike the latter, is not sensitive to the system size. We thus identify a generic feature of anisotropic active particles in three dimensions.
Sticky hard spheres, i.e., hard particles decorated with a short-ranged attractive interaction potential, constitute a relatively simple model with highly non-trivial glassy dynamics. The mode-coupling theory of the glass transition (MCT) offers a qualitative account of the complex reentrant dynamics of sticky hard spheres, but the predicted glass transition point is notoriously underestimated. Here we apply an improved first-principles-based theory, referred to as generalized mode-coupling theory (GMCT), to sticky hard spheres. This theoretical framework seeks to go beyond MCT by hierarchically expanding the dynamics in higher-order density correlation functions -- an approach that may become exact if sufficiently many correlations are taken into account. We predict the phase diagrams from the first few levels of the GMCT hierarchy and the dynamics-related critical exponents, all of which are much closer to the empirical observations than MCT. Notably, the prominent reentrant glassy dynamics, the glass-glass transition, and the higher-order bifurcation singularity classes ($A_3$ and $A_4$) of sticky hard spheres are found to be preserved within GMCT at arbitrary order. Moreover, we demonstrate that when the hierarchical order of GMCT increases, the effect of the short-ranged attractive interactions becomes more evident in the dynamics. This implies that GMCT is more sensitive to subtle microstructural differences than MCT, and that the framework provides a promising first-principles approach to systematically go beyond the MCT regime.
We combine computer simulations and analytical theory to investigate the glassy dynamics in dense assemblies of athermal particles evolving under the sole influence of self-propulsion. The simulations reveal that when the persistence time of the self-propelled particles is increased, the local structure becomes more pronounced whereas the long-time dynamics first accelerates and then slows down. These seemingly contradictory evolutions are explained by constructing a nonequilibrium mode-coupling-like theory for interacting self-propelled particles. To predict the collective dynamics the theory needs the steady state structure factor and the steady state correlations of the local velocities. It yields nontrivial predictions for the glassy dynamics of self-propelled particles in qualitative agreement with the simulations.
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