Abstract. One of the most spectacular phenomena in physics in terms of dynamical range is the glass transition and the associated slowing down of flow and relaxation with decreasing temperature. That it occurs in many different liquids seems to call for a "universal" theory. In this article, we review one such theoretical approach which is based on the concept of "frustration". Frustration in this context describes an incompatibility between extension of the locally preferred order in a liquid and tiling of the whole space. We provide a critical assessment of what has been achieved within this approach and we discuss the relation with other theories of the glass transition.
We use recently introduced three-point dynamic susceptibilities to obtain an experimental determination of the temperature evolution of the number of molecules Ncorr that are dynamically correlated during the structural relaxation of supercooled liquids. We first discuss in detail the physical content of three-point functions that relate the sensitivity of the averaged two-time dynamics to external control parameters (such as temperature or density), as well as their connection to the more standard four-point dynamic susceptibility associated with dynamical heterogeneities. We then demonstrate that these functions can be experimentally determined with good precision. We gather available data to obtain the temperature dependence of Ncorr for a large number of supercooled liquids over a wide range of relaxation time scales from the glass transition up to the onset of slow dynamics. We find that Ncorr systematically grows when approaching the glass transition. It does so in a modest manner close to the glass transition, which is consistent with an activation-based picture of the dynamics in glassforming materials. For higher temperatures, there appears to be a regime where Ncorr behaves as a power-law of the relaxation time. Finally, we find that the dynamic response to density, while being smaller than the dynamic response to temperature, behaves similarly, in agreement with theoretical expectations.
The adsorption or adhesion of large particles (proteins, colloids, cells, . . . ) at the liquid-solid interface plays an important role in many diverse applications. Despite the apparent complexity of the process, two features are particularly important: 1) the adsorption is often irreversible on experimental time scales and 2) the adsorption rate is limited by geometric blockage from previously adsorbed particles. A coarse-grained description that encompasses these two properties is provided by sequential adsorption models whose simplest example is the random sequential adsorption (RSA) process. In this article, we review the theoretical formalism and tools that allow the systematic study of kinetic and structural aspects of these sequential adsorption models. We also show how the reference RSA model may be generalized to account for a variety of experimental features including particle anisotropy, polydispersity, bulk diffusive transport, gravitational effects, surface-induced conformational and orientational change, desorption, and multilayer formation. In all cases, the significant theoretical results are presented and their accuracy (compared to computer simulation) and applicability (compared to experiment) are discussed.
We study the interplay between hysteresis and equilibrium behavior in capillary condensation of fluids in mesoporous disordered materials via a mean-field density functional theory of a disordered lattice-gas model. The approach reproduces all major features observed experimentally. We show that the simple van der Waals picture of metastability fails due to the appearance of a complex freeenergy landscape with a large number of metastable states. In particular, hysteresis can occur both with and without an underlying equilibrium transition, thermodynamic consistency is not satisfied along the hysteresis loop, and out-of-equilibrium phase transitions are possible.
We combine an analytically solvable mean-field elasto-plastic model with molecular dynamics simulations of a generic glass former to demonstrate that, depending on their preparation protocol, amorphous materials can yield in two qualitatively distinct ways. We show that well-annealed systems yield in a discontinuous brittle way, as metallic and molecular glasses do. Yielding corresponds in this case to a first-order nonequilibrium phase transition. As the degree of annealing decreases, the first-order character becomes weaker and the transition terminates in a second-order critical point in the universality class of an Ising model in a random field. For even more poorly annealed systems, yielding becomes a smooth crossover, representative of the ductile rheological behavior generically observed in foams, emulsions, and colloidal glasses. Our results show that the variety of yielding behaviors found in amorphous materials does not necessarily result from the diversity of particle interactions or microscopic dynamics but is instead unified by carefully considering the role of the initial stability of the system.
We provide a resolution of one of the long-standing puzzles in the theory of disordered systems. By reformulating the functional renormalization group for the critical behavior of the random field Ising model in a superfield formalism, we are able to follow the associated supersymmetry and its spontaneous breaking along the functional renormalization group flow. Breaking is shown to occur below a critical dimension d(DR) ≃ 5.1 and leads to a breakdown of the "dimensional reduction" property. We compute the critical exponents as a function of dimension and give evidence that scaling is described by three independent exponents.
The Stokes–Einstein and Stokes–Einstein–Debye relations hold well in nonsupercooled liquids; however, sizeable deviations from the former appear in supercooled liquids, leading to a ‘‘decoupling’’ of translational diffusion from viscosity and reorientational relaxation. We attribute this breakdown and this ‘‘decoupling’’ to the existence of structured domains in the supercooled liquid.
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