Related papers: Thermodynamic-Dynamic Interrelations in Glass-Form…
The glass transition is a long-standing unsolved problem in materials science. For polymers, our understanding of glass-formation is particularly poor due to the added complexity of chain connectivity and flexibility; structural relaxation…
Collective motion over increasing length scales is a signature of the vitrification process of liquids. We demonstrate the emergence of distinct static and dynamic length scales probed near the free surface in fully equilibrated…
Understanding and predicting the glassy dynamics of polymers remain fundamental challenges in soft matter physics. While the Elastically Collective Nonlinear Langevin Equation (ECNLE) theory has been successful in describing relaxation…
We study thermodynamic and dynamic properties of a rigid model of the fragile glass forming liquid orthoterphenyl. A system of N=343 molecules is considered in a wide range of densities and temperatures, reaching simulation times up to 1…
We present a multiscale modeling approach that integrates molecular dynamics simulations, machine learning, and the Elastically Collective Nonlinear Langevin Equation (ECNLE) theory to investigate the glass transition dynamics of polymer…
A thermodynamic measure of the fragility of liquids has recently (Ito et al ref.1) been defined in terms of the temperature dependence of the excess entropy of liquid over crystal, scaled by the excess entropy at the glass transition…
Generalized mode-coupling theory (GMCT) constitutes a systematically correctable, first-principles theory to study the dynamics of supercooled liquids and the glass transition. It is a hierarchical framework that, through the incorporation…
The emergence of the solid state in glass-forming materials upon cooling is accompanied by changes in both thermodynamic and viscoelastic properties and by a precipitous drop in fluidity. Here, we investigate changes in basic elastic…
The number of compact structures of a single condensed polymer (SCP), with similar free energies, grows exponentially with the degree of polymerization. In analogy with structural glasses (SGs), we expect that at low temperatures chain…
Supercooled liquids exhibit spatial heterogeneity in the dynamics of their fluctuating atomic arrangements. The length and time scales of the heterogeneous dynamics are central to the glass transition and influence nucleation and growth of…
The structure, thermodynamics and slow activated dynamics of the equilibrated metastable regime of glass-forming fluids remains a poorly understood problem of high theoretical and experimental interest. We apply a highly accurate…
Controversy exists regarding the possible existence of a transition between the liquid and glassy states of water. Here we use experimental measurements of the entropy, specific heat, and enthalpy of both liquid and glassy water to…
The relaxation dynamics of glass-forming systems shows a multitude of features that are absent in normal liquids, such as non-exponential relaxation and a strong temperature-dependence of the relaxation time. Connecting these dynamic…
Glass is a liquid that has lost its ability to flow. Why this particular substance undergoes its dramatic slowing down in kinetics while remaining barely distinguishable in structure from the fluid state upon cooling constitutes the central…
Using a distinguishable-particle lattice model based on void-induced dynamics, we successfully reproduce the well-known linear relation between heat capacity and temperature at very low temperatures. The heat capacity is dominated by…
We present a thermodynamic theory of the Kovacs effect based on the idea that the configurational degrees of freedom of a glass-forming material are driven out of equilibrium with the heat bath by irreversible thermal contraction and…
We explore the relationship between a machine-learned structural quantity (softness) and excess entropy in simulations of supercooled liquids. Excess entropy is known to scale well the dynamical properties of liquids, but this…
The glass transition is considered within two toys models, a mean field spin glass and a directed polymer in a correlated random potential. In the spin glass model there occurs a dynamical transition, where the system condenses in a state…
We propose a computational method to measure the configurational entropy in generic polydisperse glass-formers. In particular, our method resolves issues related to the diverging mixing entropy term due to a continuous polydispersity. The…
In this work we numerically investigate a new method for the characterization of growing length scales associated with spatially heterogeneous dynamics of glass-forming liquids. This approach, motivated by the formulation of the…