182 research outputs found
Microscopic picture of aging in SiO2
We investigate the aging dynamics of amorphous SiO2 via molecular dynamics
simulations of a quench from a high temperature T_i to a lower temperature T_f.
We obtain a microscopic picture of aging dynamics by analyzing single particle
trajectories, identifying jump events when a particle escapes the cage formed
by its neighbors, and by determining how these jumps depend on the waiting time
t_w, the time elapsed since the temperature quench to T_f. We find that the
only t_w-dependent microscopic quantity is the number of jumping particles per
unit time, which decreases with age. Similar to previous studies for fragile
glass formers, we show here for the strong glass former SiO2 that neither the
distribution of jump lengths nor the distribution of times spent in the cage
are t_w-dependent. We conclude that the microscopic aging dynamics is
surprisingly similar for fragile and strong glass formers.Comment: 4 pages, 7 figure
Self-Organized Criticality Below The Glass Transition
We obtain evidence that the dynamics of glassy systems below the glass
transition is characterized by self-organized criticality. Using molecular
dynamics simulations of a model glass-former we identify clusters of
cooperatively jumping particles. We find string-like clusters whose size is
power-law distributed not only close to T_c but for ALL temperatures below T_c,
indicating self-organized criticality which we interpret as a freezing in of
critical behavior.Comment: 4 pages, 3 figure
Aging to Equilibrium Dynamics of SiO2
Molecular dynamics computer simulations are used to study the aging dynamics
of SiO2 (modeled by the BKS model). Starting from fully equilibrated
configurations at high temperatures T_i =5000K/3760K the system is quenched to
lower temperatures T_f=2500K, 2750K, 3000K, 3250K and observed after a waiting
time t_w. Since the simulation runs are long enough to reach equilibrium at
T_f, we are able to study the transition from out-of-equilibrium to equilibrium
dynamics. We present results for the partial structure factors, for the
generalized incoherent intermediate scattering function C_q(t_w, t_w+t), and
for the mean square displacement msd(t_w,t_w+t). We conclude that there are
three different t_w regions: (I) At very short waiting times, C_q(t_w, t_w+t)
decays very fast without forming a plateau. Similarly msd(t_w,t_w+t) increases
without forming a plateau. (II) With increasing t_w a plateau develops in
C_q(t_w, t_w+t) and msd(t_w,t_w+t). For intermediate waiting times the plateau
height is independent of t_w and T_i. Time superposition applies, i.e.
C_q=C_q(t/t_r) where t_r=t_r(t_w) is a waiting time dependent decay time.
Furthermore C_q=C(q,t_w,t_w+t) scales as C_q=C(q,z(t_w,t) where z is a function
of t_w and t only, i.e. independent of q. (III) At large t_w the system reaches
equilibrium, i.e. C_q(t_w,t_w+t) and msd(t_w,t_w+t) are independent of t_w and
T_i. For C_q(t_w,t_w+t) we find that the time superposition of intermediate
waiting times (II) includes the equilibrium curve (III).Comment: 9 pages, 11 figures, submission to PR
Molecular Dynamics Computer Simulation of the Dynamics of Supercooled Silica
We present the results of a large scale computer simulation of supercooled
silica. We find that at high temperatures the diffusion constants show a
non-Arrhenius temperature dependence whereas at low temperature this dependence
is also compatible with an Arrhenius law. We demonstrate that at low
temperatures the intermediate scattering function shows a two-step relaxation
behavior and that it obeys the time temperature superposition principle. We
also discuss the wave-vector dependence of the nonergodicity parameter and the
time and temperature dependence of the non-Gaussian parameter.Comment: 5 pages, Latex, 6 postscript figure
Configurational entropy of network-forming materials
We present a computationally efficient method to calculate the
configurational entropy of network-forming materials. The method requires only
the atomic coordinates and bonds of a single well-relaxed configuration. This
is in contrast to the multiple simulations that are required for other methods
to determine entropy, such as thermodynamic integration. We use our method to
obtain the configurational entropy of well-relaxed networks of amorphous
silicon and vitreous silica. For these materials we find configurational
entropies of 1.02 kb and 0.97 kb per silicon atom, respectively, with kb the
Boltzmann constant.Comment: 4 pages, 4 figure
Citation
Transport coefficients of the TIP4P-2005 water model J. Chem. Phys. 136, 044507 (2012) Monte Carlo study of four dimensional binary hard hypersphere mixtures J. Chem. Phys. 136, 014506 (2012) Energy relaxation of intermolecular motions in supercooled water and ice: A molecular dynamics study J. Chem. Phys. 135, 244511 (2011) The role of the isothermal bulk modulus in the molecular dynamics of super-cooled liquids J. Chem. Phys. 135, 244508 (2011) Experimental evidences for molecular origin of low-Q peak in neutron/x-ray scattering of 1-alkyl-3-methylimidazolium bis(trifluoromethanesulfonyl)amide ionic liquids J. Chem. Phys. 135, 244502 (2011) Additional information on J. Chem. Phys. We present molecular dynamics simulations of a binary Lennard-Jones mixture at temperatures below the kinetic glass transition. The ''mobility'' of a particle is characterized by the amplitude of its fluctuation around its average position. The 5% particles with the largest/smallest mean amplitude are then defined as the relatively most mobile/immobile particles. We investigate for these 5% particles their spatial distribution and find them to be distributed very heterogeneously in that mobile as well as immobile particles form clusters. We suggest that this dynamic heterogeneity may be due to the fact that mobile/immobile particles are surrounded by fewer/more neighbors which form an effectively wider/narrower cage. The dependence of our results on the length of the simulation run indicates that individual particles have a characteristic mobility time scale which can be approximated via the non-Gaussian parameter
Dynamical Heterogeneities Below the Glass Transition
We present molecular dynamics simulations of a binary Lennard-Jones mixture
at temperatures below the kinetic glass transition. The ``mobility'' of a
particle is characterized by the amplitude of its fluctuation around its
average position. The 5% particles with the largest/smallest mean amplitude are
thus defined as the relatively most mobile/immobile particles. We investigate
for these 5% particles their spatial distribution and find them to be
distributed very heterogeneously in that mobile as well as immobile particles
form clusters. The reason for this dynamic heterogeneity is traced back to the
fact that mobile/immobile particles are surrounded by fewer/more neighbors
which form an effectively wider/narrower cage. The dependence of our results on
the length of the simulation run indicates that individual particles have a
characteristic mobility time scale, which can be approximated via the
non-Gaussian parameter.Comment: revtex, 10 pages, 20 postscript figure
Temperature dependence of spatially heterogeneous dynamics in a model of viscous silica
Molecular dynamics simulations are performed to study spatially heterogeneous
dynamics in a model of viscous silica above and below the critical temperature
of the mode coupling theory, . Specifically, we follow the evolution
of the dynamic heterogeneity as the temperature dependence of the transport
coefficients shows a crossover from non-Arrhenius to Arrhenius behavior when
the melt is cooled. It is demonstrated that, on intermediate time scales, a
small fraction of oxygen and silicon atoms are more mobile than expected from a
Gaussian approximation. These highly mobile particles form transient clusters
larger than that resulting from random statistics, indicating that dynamics are
spatially heterogeneous. An analysis of the clusters reveals that the mean
cluster size is maximum at times intermediate between ballistic and diffusive
motion, and the maximum size increases with decreasing temperature. In
particular, the growth of the clusters continues when the transport
coefficients follow an Arrhenius law. These findings imply that the structural
relaxation in silica cannot be understood as a statistical bond breaking
process. Though the mean cluster sizes for silica are at the lower end of the
spectrum of values reported in the literature, we find that spatially
heterogeneous dynamics in strong and fragile glass formers are similar on a
qualitative level. However, different from results for fragile liquids, we show
that correlated particle motion along quasi one-dimensional, string-like paths
is of little importance for the structural relaxation in this model of silica,
suggesting that string-like motion is suppressed by the presence of covalent
bonds.Comment: 13 pages, 11 figure
Fully Frustrated Ising System on a 3D Simple Cubic Lattice: Revisited
Using extensive Monte Carlo simulations, we clarify the critical behaviour of
the 3 dimensional simple cubic Ising Fully Frustrated system. We find two
transition temperatures and two long range ordered phases. Within the present
numerical accuracy, the transition at higher temperature is found to be second
order and we have extracted the standard critical exponent using finite size
scaling method. On the other hand, the transition at lower temperature is found
to be first order. It is argued that entropy plays a major role on determining
the low temperature state.Comment: 14 pages 14 figures iop style include
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