648 research outputs found
Molecular Dynamics Study of Orientational Cooperativity in Water
Recent experiments on liquid water show collective dipole orientation
fluctuations dramatically slower then expected (with relaxation time 50 ns)
[D. P. Shelton, Phys. Rev. B {\bf 72}, 020201(R) (2005)]. Molecular dynamics
simulations of SPC/E water show large vortex-like structure of dipole field at
ambient conditions surviving over 300 ps [J. Higo at al. PNAS, {\bf 98} 5961
(2001)]. Both results disagree with previous results on water dipoles in
similar conditions, for which autocorrelation times are a few ps. Motivated by
these recent results, we study the water dipole reorientation using molecular
dynamics simulations in bulk SPC/E water for temperatures ranging from ambient
300 K down to the deep supercooled region of the phase diagram at 210 K. First,
we calculate the dipole autocorrelation function and find that our simulations
are well-described by a stretched exponential decay, from which we calculate
the {\it orientational autocorrelation time} . Second, we define a
second characteristic time, namely the time required for the randomization of
molecular dipole orientation, the {\it self-dipole randomization time}
, which is an upper limit on ; we find that
. Third, to check if there are correlated domains
of dipoles in water which have large relaxation times compared to the
individual dipoles, we calculate the randomization time of the
site-dipole field, the net dipole moment formed by a set of molecules belonging
to a box of edge . We find that the {\it site-dipole randomization
time} for \AA, i.e.
it is shorter than the same quantity calculated for the self-dipole. Finally,
we find that the orientational correlation length is short even at low .Comment: 25 Pages, 10 figure
Is there a reentrant glass in binary mixtures?
By employing computer simulations for a model binary mixture, we show that a
reentrant glass transition upon adding a second component only occurs if the
ratio of the short-time mobilities between the glass-forming component
and the additive is sufficiently small. For , there is no
reentrant glass, even if the size asymmetry between the two components is
large, in accordance with two-component mode coupling theory. For , on the other hand, the reentrant glass is observed and reproduced only by
an effective one-component mode coupling theory.Comment: 4 pages, 3 figure
Molecular mode-coupling theory for supercooled liquids: Application to water
We present mode-coupling equations for the description of the slow dynamics
observed in supercooled molecular liquids close to the glass transition. The
mode-coupling theory (MCT) originally formulated to study the slow relaxation
in simple atomic liquids, and then extended to the analysis of liquids composed
by linear molecules, is here generalized to systems of arbitrarily shaped,
rigid molecules. We compare the predictions of the theory for the -vector
dependence of the molecular nonergodicity parameters, calculated by solving
numerically the molecular MCT equations in two different approximation schemes,
with ``exact'' results calculated from a molecular dynamics simulation of
supercooled water. The agreement between theory and simulation data supports
the view that MCT succeeds in describing the dynamics of supercooled molecular
liquids, even for network forming ones.Comment: 22 pages 4 figures Late
Reentrant glass transition in a colloid-polymer mixture with depletion attractions
Performing light scattering experiments we show that introducing short-ranged
attraction to a colloidal suspension of nearly hard spheres by addition of free
polymer produces new glass transition phenomena. We observe a dramatic
acceleration of the density fluctuations amounting to the melting of a
colloidal glass. Increasing the strength of the attractions the system freezes
into another nonergodic state sharing some qualitative features with gel states
occurring at lower colloid packing fractions. This reentrant glass transition
is in qualitative agreement with recent theoretical predictions.Comment: 14 pages, 3 figure
A view of the Galactic halo using beryllium as a time scale
Beryllium stellar abundances were suggested to be a good tracer of time in
the early Galaxy. In an investigation of its use as a cosmochronometer, using a
large sample of local halo and thick-disk dwarfs, evidence was found that in a
log(Be/H) vs. [alpha/Fe] diagram the halo stars separate into two components.
One is consistent with predictions of evolutionary models while the other is
chemically indistinguishable from the thick-disk stars. This is interpreted as
a difference in the star formation history of the two components and suggests
that the local halo is not a single uniform population where a clear
age-metallicity relation can be defined.Comment: To appear in Proceedings of the International Astronomical Union, IAU
Symposium, Volume 265, Chemical abundances in the Universe: connecting first
stars to planets, K. Cunha, M. Spite and B. Barbuy, eds. 2 Pages, 2 figure
Beryllium abundances and the formation of the halo and the thick disk
The single stable isotope of beryllium is a pure product of cosmic-ray
spallation in the ISM. Assuming that the cosmic-rays are globally transported
across the Galaxy, the beryllium production should be a widespread process and
its abundance should be roughly homogeneous in the early-Galaxy at a given
time. Thus, it could be useful as a tracer of time. In an investigation of the
use of Be as a cosmochronometer and of its evolution in the Galaxy, we found
evidence that in a log(Be/H) vs. [alpha/Fe] diagram the halo stars separate
into two components. One is consistent with predictions of evolutionary models
while the other is chemically indistinguishable from the thick-disk stars. This
is interpreted as a difference in the star formation history of the two
components and suggests that the local halo is not a single uniform population
where a clear age-metallicity relation can be defined. We also found evidence
that the star formation rate was lower in the outer regions of the thick disk,
pointing towards an inside-out formation.Comment: 6 pages, 5 figures, To appear in the Proceedings of IAU Symp. 268 -
Light Elements in the Universe (C. Charbonnel, M. Tosi, F. Primas, C.
Chiappini, eds
Dynamics in a supercooled molecular liquid: Theory and Simulations
We report extensive simulations of liquid supercooled states for a simple
three-sites molecular model, introduced by Lewis and Wahnstr"om [L. J. Lewis
and G. Wahnstr"om, Phys. Rev. E 50, 3865 (1994)] to mimic the behavior of
ortho-terphenyl. The large system size and the long simulation length allow to
calculate very precisely --- in a large q-vector range --- self and collective
correlation functions, providing a clean and simple reference model for
theoretical descriptions of molecular liquids in supercooled states. The time
and wavevector dependence of the site-site correlation functions are compared
with detailed predictions based on ideal mode-coupling theory, neglecting the
molecular constraints. Except for the wavevector region where the dynamics is
controlled by the center of mass (around 9 nm-1), the theoretical predictions
compare very well with the simulation data.
Equilibration times in numerical simulation of structural glasses: Comparing parallel tempering and conventional molecular dynamics
Generation of equilibrium configurations is the major obstacle for numerical
investigation of the slow dynamics in supercooled liquid states. The parallel
tempering (PT) technique, originally proposed for the numerical equilibration
of discrete spin-glass model configurations, has recently been applied in the
study of supercooled structural glasses. We present an investigation of the
ability of parallel tempering to properly sample the liquid configuration space
at different temperatures, by mapping the PT dynamics into the dynamics of the
closest local potential energy minima (inherent structures). Comparing the PT
equilibration process with the standard molecular dynamics equilibration
process we find that the PT does not increase the speed of equilibration of the
(slow) configurational degrees of freedom.Comment: 5 pages, 3 figure
Reorientational relaxation of a linear probe molecule in a simple glassy liquid
Within the mode-coupling theory (MCT) for the evolution of structural
relaxation in glass-forming liquids, correlation functions and susceptibility
spectra are calculated characterizing the rotational dynamics of a top-down
symmetric dumbbell molecule, consisting of two fused hard spheres immersed in a
hard-sphere system. It is found that for sufficiently large dumbbell
elongations, the dynamics of the probe molecule follows the same universal
glass-transition scenario as known from the MCT results of simple liquids. The
-relaxation process of the angular-index-j=1 response is stronger,
slower and less stretched than the one for j=2, in qualitative agreement with
results found by dielectric-loss and depolarized-light-scattering spectroscopy
for some supercooled liquids. For sufficiently small elongations, the
reorientational relaxation occurs via large-angle flips, and the standard
scenario for the glass-transition dynamics is modified for odd-j responses due
to precursor phenomena of a nearby type-A MCT transition. In this case, a major
part of the relaxation outside the transient regime is described qualitatively
by the -relaxation scaling laws, while the -relaxation scaling
law is strongly disturbed.Comment: 40 pages. 10 figures as GIF-files, to be published in Phys. Rev.
Test of the semischematic model for a liquid of linear molecules
We apply to a liquid of linear molecules the semischematic mode-coupling
model, previously introduced to describe the center of mass (COM) slow dynamics
of a network-forming molecular liquid. We compare the theoretical predictions
and numerical results from a molecular dynamics simulation, both for the time
and the wave-vector dependence of the COM density-density correlation function.
We discuss the relationship between the presented analysis and the results from
an approximate solution of the equations from molecular mode-coupling theory
[R. Schilling and T. Scheidsteger, Phys. Rev. E 56 2932 (1997)].Comment: Revtex, 10 pages, 4 figure
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