相关论文: Configurational Entropy and Diffusivity of Superco…
We present examples of systems whose configurational entropy $S_{\text{conf}}$ can never reach zero and is instead limited from below by the entropy of mixing $S_{\text{mix}}$ of the corresponding ideal gas. We use $S_{\text{conf}}$ defined…
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,…
In the present article we carry out a molecular dynamics study of the core-softened system and show that the existence of the water-like anomalies in this system depends on the trajectory in $P-\rho-T$ space along which the behavior of the…
Supercooled water exhibits a breakdown of the Stokes-Einstein relation between the diffusion constant $D$ and the alpha relaxation time $\tau_{\alpha}$. For water simulated with the TIP5P and ST2 potentials, we find that the temperature of…
We study tagged particle diffusion at large packing fractions, for a model of particles interacting with a generalized Lennard-Jones 2n-n potential, with large n. The resulting short-range potential mimics interactions in colloidal systems.…
We investigate the spatially heterogeneous dynamics in the SPC/E model of water by using molecular dynamics simulations. We relate the average mass $n^*$ of mobile particle clusters to the diffusion constant and the configurational entropy.…
We construct a configurational entropy measure in functional space. We apply it to several nonlinear scalar field models featuring solutions with spatially-localized energy, including solitons and bounces in one spatial dimension, and…
It is shown that the fraction f of imaginary frequency instantaneous normal modes (INM) may be defined and calculated in a random energy model(REM) of liquids. The configurational entropy S and the averaged hopping rate among the states R…
We introduce an exactly solvable lattice model that reveals a universal finite-size scaling law for configurational entropy driven purely by geometry. Using exact enumeration via Burnside's lemma, we compute the entropy for diverse 1D, 2D,…
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…
We use rigorous nonequilibrium thermodynamic arguments to establish that (i) the nonequilibrium entropy S(T_{0}) of any system is bounded below by the experimentally (calorimetrically) determined entropy S_{expt}(T_{0}), (ii)…
Configurational entropy is an important factor in the free energy change of many macromolecular recognition and binding processes, and has been intensively studied. Despite great progresses that have been made, the global sampling remains…
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…
We present molecular dynamics simulations of the SPC/E model of water to probe the dynamic properties at temperatures from 350 K down to 190 K and pressures from 2.5GPa (25kbar) down to -300MPa (-3kbar). We compare our results with those…
We define the entropy S and uncertainty function of a squeezed system interacting with a thermal bath, and study how they change in time by following the evolution of the reduced density matrix in the influence functional formalism. As…
Twenty years ago Poole et al. (Nature 360, 324, 1992) suggested that the anomalous properties of supercooled water may be caused by a critical point that terminates a line of liquid-liquid separation of lower-density and higher-density…
We analyze the nature of the structural order established in liquid TIP4P water in the framework provided by the multi-particle correlation expansion of the statistical entropy. Different regimes are mapped onto the phase diagram of the…
We report the diffusion coefficient and viscosity of popular rigid water models: Two non polarizable ones (SPC/E with 3 sites, and TIP4P/2005 with 4 sites) and a polarizable one (Dang-Chang, 4 sites). We exploit the dependence of the…
Most methods for estimating configurational entropy from molecular simulation data yield upper limits except for harmonic systems where they are exact. Problems arise at diffusive systems and the presence of conformational transitions.…
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…