2,068 research outputs found
Some Finite Size Effects in Simulations of Glass Dynamics
We present the results of a molecular dynamics computer simulation in which
we investigate the dynamics of silica. By considering different system sizes,
we show that in simulations of the dynamics of this strong glass former
surprisingly large finite size effects are present. In particular we
demonstrate that the relaxation times of the incoherent intermediate scattering
function and the time dependence of the mean squared displacement are affected
by such finite size effects. By compressing the system to high densities, we
transform it to a fragile glass former and find that for that system these
types of finite size effects are much weaker.Comment: 12 pages of RevTex, 4 postscript figures available from W. Ko
The viscous slowing down of supercooled liquids as a temperature-controlled superArrhenius activated process: a description in terms of frustration-limited domains
We propose that the salient feature to be explained about the glass
transition of supercooled liquids is the temperature-controlled superArrhenius
activated nature of the viscous slowing down, more strikingly seen in
weakly-bonded, fragile systems. In the light of this observation, the relevance
of simple models of spherically interacting particles and that of models based
on free-volume congested dynamics are questioned. Finally, we discuss how the
main aspects of the phenomenology of supercooled liquids, including the
crossover from Arrhenius to superArrhenius activated behavior and the
heterogeneous character of the relaxation, can be described by an
approach based on frustration-limited domains.Comment: 13 pages, 4 figures, accepted in J. Phys.: Condensed Matter,
proceedings of the Trieste workshop on "Unifying Concepts in Glass Physics
Spatially heterogeneous dynamics and dynamic facilitation in a model of viscous silica
Performing molecular dynamics simulations, we find that the structural
relaxation dynamics of viscous silica, the prototype of a strong glass former,
are spatially heterogeneous and cannot be understood as a statistical bond
breaking process. Further, we show that high particle mobility predominantly
propagates continuously through the melt, supporting the concept of dynamic
facilitation emphasized in recent theoretical work.Comment: 4 pages, 4 figure
Molecular Dynamics Simulations of a Pressure-induced Glass Transition
We simulate the compression of a two-component Lennard-Jones liquid at a
variety of constant temperatures using a molecular dynamics algorithm in an
isobaric-isothermal ensemble. The viscosity of the liquid increases with
pressure, undergoing a broadened transition into a structurally arrested,
amorphous state. This transition, like the more familiar one induced by
cooling, is correlated with a significant increase in icosahedral ordering. In
fact, the structure of the final state, as measured by an analysis of the
bonding, is essentially the same in the glassy, frozen state whether produced
by squeezing or by cooling under pressure. We have computed an effective
hard-sphere packing fraction at the transition, defining the transition
pressure or temperature by a cutoff in the diffusion constant, analogous to the
traditional laboratory definition of the glass transition by an arbitrary, low
cutoff in viscosity. The packing fraction at this transition point is not
constant, but is consistently higher for runs compressed at higher temperature.
We show that this is because the transition point defined by a constant cutoff
in the diffusion constant is not the same as the point of structural arrest, at
which further changes in pressure induce no further structural changes, but
that the two alternate descriptions may be reconciled by using a thermally
activated cutoff for the diffusion constant. This enables estimation of the
characteristic activation energy for diffusion at the point of structural
arrest.Comment: Latex using Revtex macro
Liquid-liquid phase transition in Stillinger-Weber silicon
It was recently demonstrated that the Stillinger-Weber silicon undergoes a
liquid-liquid first-order phase transition deep into the supercooled region
(Sastry and Angell, Nature Materials 2, 739 (2003)). Here we study the effects
of perturbations on this phase transition. We show that the order of the
liquid-liquid transition changes with negative pressure. We also find that the
liquid-liquid transition disappears when the three-body term of the potential
is strengthened by as little as 5 %. This implies that the details of the
potential could affect strongly the nature and even the existence of the
liquid-liquid phase.Comment: 13 page
The Ising M-p-spin mean-field model for the structural glass: continuous vs. discontinuous transition
The critical behavior of a family of fully connected mean-field models with
quenched disorder, the Ising spin glass, is analyzed, displaying a
crossover between a continuous and a random first order phase transition as a
control parameter is tuned. Due to its microscopic properties the model is
straightforwardly extendable to finite dimensions in any geometry.Comment: 10 pages, 1 figure, 1 tabl
Two-Gaussian excitations model for the glass transition
We develop a modified "two-state" model with Gaussian widths for the site
energies of both ground and excited states, consistent with expectations for a
disordered system. The thermodynamic properties of the system are analyzed in
configuration space and found to bridge the gap between simple two state models
("logarithmic" model in configuration space) and the random energy model
("Gaussian" model in configuration space). The Kauzmann singularity given by
the random energy model remains for very fragile liquids but is suppressed or
eliminated for stronger liquids. The sharp form of constant volume heat
capacity found by recent simulations for binary mixed Lennard Jones and soft
sphere systems is reproduced by the model, as is the excess entropy and heat
capacity of a variety of laboratory systems, strong and fragile. The ideal
glass in all cases has a narrow Gaussian, almost invariant among molecular and
atomic glassformers, while the excited state Gaussian depends on the system and
its width plays a role in the thermodynamic fragility. The model predicts the
existence of first-order phase transition for fragile liquids.Comment: 12 pages, 12 figure
Microscopic theory of network glasses
A molecular theory of the glass transition of network forming liquids is
developed using a combination of self-consistent phonon and liquid state
approaches. Both the dynamical transition and the entropy crisis characteristic
of random first order transitions are mapped out as a function of the degree of
bonding and the density. Using a scaling relation for a soft-core model to
crudely translate the densities into temperatures, the theory predicts that the
ratio of the dynamical transition temperature to the laboratory transition
temperature rises as the degree of bonding increases, while the Kauzmann
temperature falls relative to the laboratory transition. These results indicate
why highly coordinated liquids should be "strong" while van der Waals liquids
without coordination are "fragile".Comment: slightly revised version that has been accepted for publication in
Phys. Rev. Let
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