Theory of structural glasses and supercooled liquids.

  title={Theory of structural glasses and supercooled liquids.},
  author={Vassiliy Lubchenko and Peter G. Wolynes},
  journal={Annual review of physical chemistry},
We review the random first-order transition theory of the glass transition, emphasizing the experimental tests of the theory. Many distinct phenomena are quantitatively predicted or explained by the theory, both above and below the glass transition temperature T(g). These include the following: the viscosity catastrophe and heat-capacity jump at T(g), and their connection; the nonexponentiality of relaxations and their correlation with the fragility; dynamic heterogeneity in supercooled liquids… 
Dynamical heterogeneity of the glassy state.
Dynamical heterogeneities in equilibrated supercooled liquids and in the nonequilibrium glassy state are compared within the framework of the random first order transition theory to explain in a unified way recent experimental observations that have been interpreted as coming from there being two distinct equilibration mechanisms in glasses.
Liquid state elasticity and the onset of activated transport in glass formers.
The crossover temperature to activated transport in glass-forming liquids can be predicted using their finite-frequency elastic constants and the fusion entropy using the notion that, at the crossover, the "Lindemann ratio" of this vibrational displacement to the corresponding lattice spacing is nearly system-independent.
On the ergodicity of supercooled molecular glass-forming liquids at the dynamical arrest: the o-terphenyl case
The experimental data give evidence that the time scales of the primary (α) and this secondary relaxations are correlated, and a comparison with recent PCS experiments in a colloidal system confirms the primary role of the dynamical crossover in the physics of theynamical arrest.
Cooperative motions in supercooled liquids and glasses
Why glasses behave like solids in the absence of their having any long range structural order, is a fundamental problem of statistical physics, one that has been actively researched for more than 80
Non-monotonic pressure dependence of the dynamics of soft glass-formers at high compressions
In molecular dynamics simulations of soft glass-formers interacting via repulsions, we find that the glass transition temperature, dynamical heterogeneity, and glass fragility reach their maxima at
Glass Transition in Supercooled Liquids with Medium-Range Crystalline Order.
This study performs extensive molecular dynamics simulations of a number ofGlass forming liquids and shows that the static and dynamic properties of glasses with MRCO are different from those of other glass forming liquids with no predominant local order.
Molecular Theories of Segmental Dynamics and Mechanical Response in Deeply Supercooled Polymer Melts and Glasses
We review recent progress in developing statistical mechanical theories for the slow activated segmental dynamics and mechanical response of deeply supercooled polymer melts and glasses. The focus is
Kovacs Effect and the Relation Between Glasses and Supercooled Liquids
In this note we revisit the Kovacs effect, concerning the way in which the volume of a glass-forming liquid, which has been driven out of equilibrium, changes with time while the system evolves
Dynamical Theory of Segmental Relaxation and Emergent Elasticity in Supercooled Polymer Melts
We generalize the force-level Elastically Collective Nonlinear Langevin Equation theory of supercooled molecular liquid dynamics to polymer melts based on mapping chains to disconnected and
Segmental dynamics in polymers: from cold melts to ageing and stressed glasses
Current progress in developing statistical mechanical theories of supercooled polymer melts and glasses includes two configurational entropy theories, a percolated free volume distribution model, and the activated barrier hopping nonlinear Langevin theory.


Microscopic theory of heterogeneity and nonexponential relaxations in supercooled liquids.
A microscopic approach derives a relation between the departure from Debye relaxation as characterized by the beta value of a stretched exponential response function, phi(t) = e(-(t/tau(KWW))beta), and the fragility of the liquid.
Theory of aging in structural glasses.
The resulting microscopic theory of aging makes contact with the Nayaranaswamy-Moynihan-Tool nonlinear relaxation formalism and the Hodge-Scherer extrapolation of the Adam-Gibbs formula, but deviations from both approaches are predicted and shown to be consistent with experiment.
Fragilities of liquids predicted from the random first order transition theory of glasses.
  • X. Xia, P. Wolynes
  • Physics
    Proceedings of the National Academy of Sciences of the United States of America
  • 2000
The wide variety of kinetic behavior in liquids of quite disparate chemical nature reflects quantitative rather than qualitative differences in their energy landscapes.
Droplets and the configurational entropy crisis for random first-order transitions
We consider the effect of droplet excitations in the random first-order transition theory of glasses on the configurational entropy. The contribution of these excitations is estimated both at and
Correlation of fragility of supercooled liquids with elastic properties of glasses.
It is argued that the ratio of the moduli controls the high-temperature activation energy of the structural relaxation and in this way affects the fragility.
Entropy and Fragility in Supercooling Liquids
  • C. Angell
  • Physics
    Journal of research of the National Institute of Standards and Technology
  • 1997
It is shown how the relaxation expression of Adam and Gibbs qualitatively accounts for most of the phenomenology of liquid and polymeric glassformers including the strong/fragile liquid pattern, and the behavior of non-ergodic systems.
Dynamics of glass-forming liquids. V. On the link between molecular dynamics and configurational entropy
We compare dielectric relaxation τ(T) data of several low molecular weight glass-forming liquids with the predictions of the Adam–Gibbs theory using experimental data for the configurational entropy
Thermodynamic-kinetic correlations in supercooled liquids: a critical survey of experimental data and predictions of the random first-order transition theory of glasses.
The quantitative predictions of alpha-relaxation activation barriers provided by the theory of glasses based on random first-order transitions are compared with the experimental results for 44 substances and the agreement found between the predicted activation energies near T(g) and experiment is excellent.
Microscopic theory of network glasses.
A theory of the glass transition of network liquids is developed using self-consistent phonon and liquid state approaches, predicting the ratio of the dynamical transition temperature to the laboratory transition temperature rises as the degree of bonding increases, while the Kauzmann temperature falls.