771 research outputs found
On Static and Dynamic Heterogeneities in Water
We analyze differences in dynamics and in properties of the sampled potential
energy landscape between different equilibrium trajectories, for a system of
rigid water molecules interacting with a two body potential. On entering in the
supercooled region, differences between different realizations enhance and
survive even when particles have diffused several time their average distance.
We observe a strong correlation between the mean square displacement of the
individual trajectories and the average energy of the sampled landscape
Liquid stability in a model for ortho-terphenyl
We report an extensive study of the phase diagram of a simple model for
ortho-terphenyl, focusing on the limits of stability of the liquid state.
Reported data extend previous studies of the same model to both lower and
higher densities and to higher temperatures. We estimate the location of the
homogeneous liquid-gas nucleation line and of the spinodal locus. Within the
potential energy landscape formalism, we calculate the distributions of depth,
number, and shape of the potential energy minima and show that the statistical
properties of the landscape are consistent with a Gaussian distribution of
minima over a wide range of volumes. We report the volume dependence of the
parameters entering in the Gaussian distribution (amplitude, average energy,
variance). We finally evaluate the locus where the configurational entropy
vanishes, the so-called Kauzmann line, and discuss the relative location of the
spinodal and Kauzmann loci.Comment: RevTeX 4, 8 pages, 8 eps figure
Energy landscape of a simple model for strong liquids
We calculate the statistical properties of the energy landscape of a minimal
model for strong network-forming liquids. Dynamics and thermodynamic properties
of this model can be computed with arbitrary precision even at low
temperatures. A degenerate disordered ground state and logarithmic statistics
for the energy distribution are the landscape signatures of strong liquid
behavior. Differences from fragile liquid properties are attributed to the
presence of a discrete energy scale, provided by the particle bonds, and to the
intrinsic degeneracy of topologically disordered networks.Comment: Revised versio
Non-Gaussian energy landscape of a simple model for strong network-forming liquids: accurate evaluation of the configurational entropy
We present a numerical study of the statistical properties of the potential
energy landscape of a simple model for strong network-forming liquids. The
model is a system of spherical particles interacting through a square well
potential, with an additional constraint that limits the maximum number of
bonds, , per particle. Extensive simulations have been carried out
as a function of temperature, packing fraction, and . The dynamics
of this model are characterized by Arrhenius temperature dependence of the
transport coefficients and by nearly exponential relaxation of dynamic
correlators, i.e. features defining strong glass-forming liquids. This model
has two important features: (i) landscape basins can be associated with bonding
patterns; (ii) the configurational volume of the basin can be evaluated in a
formally exact way, and numerically with arbitrary precision. These features
allow us to evaluate the number of different topologies the bonding pattern can
adopt. We find that the number of fully bonded configurations, i.e.
configurations in which all particles are bonded to neighbors, is
extensive, suggesting that the configurational entropy of the low temperature
fluid is finite. We also evaluate the energy dependence of the configurational
entropy close to the fully bonded state, and show that it follows a logarithmic
functional form, differently from the quadratic dependence characterizing
fragile liquids. We suggest that the presence of a discrete energy scale,
provided by the particle bonds, and the intrinsic degeneracy of fully bonded
disordered networks differentiates strong from fragile behavior.Comment: Final version. Journal of Chemical Physics 124, 204509 (2006
Configuration space connectivity across the fragile to strong transition in silica
We present a numerical analysis for SiO_2 of the fraction of diffusive
direction f_diff for temperatures T on both sides of the fragile-to-strong
crossover. The T-dependence of f_diff clearly reveals this change in dynamical
behavior. We find that for T above the crossover (fragile region) the system is
always close to ridges of the potential energy surface (PES), while below the
crossover (strong region), the system mostly explores the PES local minima.
Despite this difference, the power law dependence of f_diff on the diffusion
constant, as well as the power law dependence of f_diff on the configurational
entropy, shows no change at the fragile to strong crossover
Maximum Valency Lattice Gas Models
We study lattice gas models with the imposition of a constraint on the
maximum number of bonds (nearest neighbor interactions) that particles can
participate in. The critical parameters, as well as the coexistence region are
studied using the mean field approximation and the Bethe-Peierls approximation.
We find that the reduction of the number of interactions suppresses the
temperature-density region where the liquid and gas phases coexist. We confirm
these results from simulations using the histogram reweighting method employing
grand Canonical Monte Carlo simulations
Mode-coupling theory predictions for a limited valency attractive square-well model
Recently we have studied, using numerical simulations, a limited valency
model, i.e. an attractive square well model with a constraint on the maximum
number of bonded neighbors. Studying a large region of temperatures and
packing fractions , we have estimated the location of the liquid-gas
phase separation spinodal and the loci of dynamic arrest, where the system is
trapped in a disordered non-ergodic state. Two distinct arrest lines for the
system are present in the system: a {\it (repulsive) glass} line at high
packing fraction, and a {\it gel} line at low and . The former is
essentially vertical (-controlled), while the latter is rather horizontal
(-controlled) in the plane. We here complement the molecular
dynamics results with mode coupling theory calculations, using the numerical
structure factors as input. We find that the theory predicts a repulsive glass
line -- in satisfactory agreement with the simulation results -- and an
attractive glass line which appears to be unrelated to the gel line.Comment: 12 pages, 6 figures. To appear in J. Phys. Condens. Matter, special
issue: "Topics in Application of Scattering Methods for Investigation of
Structure and Dynamics of Soft Condensed Matter", Fiesole, November 200
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