73 research outputs found
Phase diagram of silica from computer simulation
We evaluate the phase diagram of the ``BKS'' potential [Van Beest, Kramer and
van Santen, Phys. Rev. Lett. 64, 1955 (1990)], a model of silica widely used in
molecular dynamics (MD) simulations. We conduct MD simulations of the liquid,
and three crystals (beta-quartz, coesite and stishovite) over wide ranges of
temperature and density, and evaluate the total Gibbs free energy of each
phase. The phase boundaries are determined by the intersection of these free
energy surfaces. Not unexpectedly for a classical pair potential, our results
reveal quantitative discrepancies between the locations of the BKS and real
silica phase boundaries. At the same time, we find that the topology of the
real phase diagram is reproduced, confirming that the BKS model provides a
satisfactory qualitative description of a silica-like material. We also compare
the phase boundaries with the locations of liquid-state thermodynamic anomalies
identified in previous studies of the BKS model.Comment: 7 pages, 7 figure
Landscapes, dynamic heterogeneity and kinetic facilitation in a simple off-lattice model
We present a simple off-lattice hard-disc model that exhibits glassy
dynamics. The inherent structures are enumerated exactly, transitions between
metabasins are well understood, and the particle configurations that act to
facilitate dynamics are easily identified. The model readily maps to a coarse
grained dynamic facilitation description.Comment: 5 pages, 5 figures, submitted to PR
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
A Family of Tunable Spherically-Symmetric Potentials that Span the Range from Hard Spheres to Water-like Behavior
We investigate the equation of state, diffusion coefficient, and structural
order of a family of spherically-symmetric potentials consisting of a hard core
and a linear repulsive ramp. This generic potential has two characteristic
length scales: the hard and soft core diameters. The family of potentials is
generated by varying their ratio, . We find negative thermal expansion
(thermodynamic anomaly) and an increase of the diffusion coefficient upon
isothermal compression (dynamic anomaly) for . As in water,
the regions where these anomalies occur are nested domes in the () or
() planes, with the thermodynamic anomaly dome contained entirely within
the dynamic anomaly dome. We calculate translational and orientational order
parameters ( and ), and project equilibrium state points onto the () plane, or order map. The order map evolves from water-like behavior to
hard-sphere-like behavior upon varying between 4/7 and 6/7. Thus, we
traverse the range of liquid behavior encompassed by hard spheres ()
and water-like () with a family of tunable
spherically-symmetric potentials by simply varying the ratio of hard to
soft-core diameters. Although dynamic and thermodynamic anomalies occur almost
across the entire range , water-like structural anomalies
(i.e., decrease in both and upon compression and strictly correlated
and in the anomalous region) occur only around .
Water-like anomalies in structure, dynamics and thermodynamics arise solely due
to the existence of two length scales, orientation-dependent interactions being
absent by design.Comment: total 21 pages, 6 figure
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
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
Effect of bond lifetime on the dynamics of a short-range attractive colloidal system
We perform molecular dynamics simulations of short-range attractive colloid
particles modeled by a narrow (3% of the hard sphere diameter) square well
potential of unit depth. We compare the dynamics of systems with the same
thermodynamics but different bond lifetimes, by adding to the square well
potential a thin barrier at the edge of the attractive well. For permanent
bonds, the relaxation time diverges as the packing fraction
approaches a threshold related to percolation, while for short-lived bonds, the
-dependence of is more typical of a glassy system. At intermediate
bond lifetimes, the -dependence of is driven by percolation at low
, but then crosses over to glassy behavior at higher . We also
study the wavevector dependence of the percolation dynamics.Comment: Revised; 9 pages, 9 figure
Liquid Polymorphism and Double Criticality in a Lattice Gas Model
We analyze the possible phase diagrams of a simple model for an associating
liquid proposed previously. Our two-dimensional lattice model combines
oreintati onal ice-like interactions and \"{}Van der Waals\"{} interactions
which may be repulsive, and in this case represent a penalty for distortion of
hydrogen bonds in the presence of extra molecules. These interactions can be
interpreted in terms of two competing distances, but not necessarily soft-core.
We present mean -field calculations and an exhaustive simulation study for
different parameters which represent relative strength of the bonding
interaction to the energy penalty for its distortion. As this ratio decreases,
a smooth disappearance of the doubl e criticality occurs. Possible connections
to liquid-liquid transitions of molecul ar liquids are suggested
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