Lifetime of dynamic heterogeneity in strong and fragile kinetically constrained spin models

Kinetically constrained spin models are schematic coarse-grained models for the glass transition which represent an efficient theoretical tool to study detailed spatio-temporal aspects of dynamic heterogeneity in supercooled liquids. Here, we study how spatially correlated dynamic domains evolve with time and compare our results to various experimental and numerical investigations. We find that strong and fragile models yield different results. In particular, the lifetime of dynamic heterogeneity remains constant and roughly equal to the alpha relaxation time in strong models, while it increases more rapidly in fragile models when the glass transition is approached.Comment: Submitted to the proceedings of the 6th EPS Liquid Matter Conference, Utrecht 2-6 July 200

Coarse-grained microscopic model of glass formers

We introduce a coarse-grained model for atomic glass formers. Its elements are physically motivated local microscopic dynamical rules parameterized by observables. Results of the model are established and used to interpret the measured behaviors of supercooled fluids approaching glass transitions. The model predicts the presence of a crossover from hierarchical super-Arrhenius dynamics at short length scales to diffusive Arrhenius dynamics at large length scales. This prediction distinguishes our model from other theories of glass formers and can be tested by experiment.Comment: 5 pages, 5 figure

Space-time Thermodynamics of the Glass Transition

We consider the probability distribution for fluctuations in dynamical action and similar quantities related to dynamic heterogeneity. We argue that the so-called "glass transition" is a manifestation of low action tails in these distributions where the entropy of trajectory space is sub-extensive in time. These low action tails are a consequence of dynamic heterogeneity and an indication of phase coexistence in trajectory space. The glass transition, where the system falls out of equilibrium, is then an order-disorder phenomenon in space-time occurring at a temperature T_g which is a weak function of measurement time. We illustrate our perspective ideas with facilitated lattice models, and note how these ideas apply more generally.Comment: 5 pages, 4 figure

Two-step devitrification of ultrastable glasses

The discovery of ultrastable glasses has raised novel challenges about glassy systems. Recent experiments studied the macroscopic devitrification of ultrastable glasses into liquids upon heating but lacked microscopic resolution. We use molecular dynamics simulations to analyse the kinetics of this transformation. In the most stable systems, devitrification occurs after a very large time, but the liquid emerges in two steps. At short times, we observe the rare nucleation and slow growth of isolated droplets containing a liquid maintained under pressure by the rigidity of the surrounding glass. At large times, pressure is released after the droplets coalesce into large domains, which accelerates devitrification. This two-step process produces pronounced deviations from the classical Avrami kinetics and explains the emergence of a giant lengthscale characterising the devitrification of bulk ultrastable glasses. Our study elucidates the nonequilibrium kinetics of glasses following a large temperature jump, which differs from both equilibrium relaxation and aging dynamics, and will guide future experimental studies

Dynamics of glass-forming liquids. XVI. Observation of ultrastable glass transformation via dielectric spectroscopy

The transformation of vapor-deposited ultrastable glasses of indomethacin (IMC) into the supercooled liquid state near Tg is monitored by means of dielectric spectroscopy. Films with thickness between 400 and 800 nm are deposited on differential interdigitated electrode cells and their loss profiles are measured during isothermal annealing using a dual-channel impedance technique for frequencies between 0.03 and 100 Hz. All dielectric loss spectra observed during the transformation process can be explained by a volume fraction of the supercooled liquid that increases linearly with time. From the early stages of the transformation to the liquid that is formed via complete annealing of the ultrastable glass, the average dielectric relaxation time as well as the distribution of relaxation times of the liquid component are identical to those of the conventional liquid obtained by cooling the melt. The dependence of the transformation rate on the film thickness is consistent with a growth front mechanism for the direct conversion from the ultrastable glass to the equilibrium supercooled liquid. We conclude that the IMC liquid recovered from the ultrastable glass is structurally and dynamically identical to the conventional supercooled state

Properties of cage rearrangements observed near the colloidal glass transition

We use confocal microscopy to study the motions of particles in concentrated colloidal systems. Near the glass transition, diffusive motion is inhibited, as particles spend time trapped in transient ``cages'' formed by neighboring particles. We measure the cage sizes and lifetimes, which respectively shrink and grow as the glass transition approaches. Cage rearrangements are more prevalent in regions with lower local concentrations and higher disorder. Neighboring rearranging particles typically move in parallel directions, although a nontrivial fraction move in anti-parallel directions, usually from pairs of particles with initial separations corresponding to the local maxima and minima of the pair correlation function $g(r)$, respectively.Comment: 5 pages, 4 figures; text & figures revised in v