Related papers: Configurational entropy of polydisperse supercoole…
Classical particle systems characterized by continuous size polydispersity, such as colloidal materials, are not straightforwardly described using statistical mechanics, since fundamental issues may arise from particle distinguishability.…
The configurational entropy is one of the most important thermodynamic quantities characterizing supercooled liquids approaching the glass transition. Despite decades of experimental, theoretical, and computational investigation, a widely…
The configurational entropy is an indispensable tool to describe super-cooled liquids near the glass transition. Its calculation requires the enumeration of the basins in the potential energy landscape and when available, it reveals a…
Computer simulations have been employed in recent years to evaluate the configurational entropy changes in model glass-forming liquids. We consider two methods, both of which involve the calculation of the `intra-basin' entropy as a means…
We compute the low-temperature configurational entropy of a two-dimensional supercooled liquid. Our method, based on a higher-dimensional version of the Grassberger--Procaccia algorithm, can be implemented in a manner that is entirely…
The configurational entropy is among the key observables to characterize experimentally the formation of a glass. Physically, it quantifies the multiplicity of metastable states in which an amorphous material can be found at a given…
Liquids relax extremely slowly upon approaching the glass state. One explanation is that an entropy crisis, due to the rarefaction of available states, makes it increasingly arduous to reach equilibrium in that regime. Validating this…
We combine population annealing Monte Carlo and several thermodynamic integration techniques to measure equilibrium vibrational and configurational entropies in the metastable fluid regime beyond the dynamic glass transition. We obtain…
Polydisperse systems are commonly encountered when dealing with soft matter in general or any non simple fluid. Yet their treatment within the framework of statistical thermodynamics is a delicate task as the latter has been essentially…
It is often stated that if one is presented with a snapshot of the positions of the molecules of a glass and one of a liquid, one is unable to tell the difference. Here we argue instead that given several such snapshots taken over a…
The inherent structure approach, wherein thermodynamic and structural changes in glass forming liquids are analyzed in terms of local potential energy minima that the liquid samples, has recently been applied extensively to the study of…
We applied an efficient methodology to separate vibrational and configurational entropies in bulk metallic glasses by means of molecular dynamics simulation based on a combination of non-equilibrium adiabatic switching and reversible…
We explore the nature of glass-formation in variable spatial dimensionality ($d$) based on the generalized entropy theory, a synthesis of the Adam-Gibbs model with direct computation of the configurational entropy of polymer fluids using an…
Diffusivity, a measure for how rapidly a fluid self-mixes, shows an intimate, but seemingly fragmented, connection to thermodynamics. On one hand, the "configurational" contribution to entropy (related to the number of mechanically-stable…
We introduce an experimental method of assessing the vibrational and configurational components of the excess entropy of a liquid over crystal, based on a joined investigation of dynamic and thermodynamic properties as a function of…
We connect the configurational entropy of a liquid to the geometrical properties of its local energy landscape, using a high-temperature expansion. It is proposed that correlations between local structures arises from their overlap and,…
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…
The length-scale dependence of the dynamic entropy is studied in a molecular dynamics simulation of a binary Lennard-Jones liquid above the mode-coupling critical temperature $T_c$. A number of methods exist for estimating the entropy of…
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…
By taking advantage of the molecular weight dependence of the glass transition of polymers and their ability to form perfectly miscible blends, we propose a way to modify the fragility of a system, from fragile to strong, keeping the same…