73 research outputs found
Direct observation of molecular cooperativity near the glass transition
We describe direct observations of molecular cooperativity near the glass
transition in poly-vinyl-acetate (PVAc), through nanometer-scale probing of
dielectric fluctuations. Molecular clusters switched spontaneously between two
to four distinct configurations, producing complex random-telegraph-signals
(RTS). Analysis of the RTS and their power spectra shows that individual
clusters exhibit both transient dynamical heterogeneity and non-exponential
kinetics.Comment: 14 pages pdf, need Acrobat Reade
Origin of non-exponential relaxation in a crystalline ionic conductor: a multi-dimensional 109Ag NMR study
The origin of the non-exponential relaxation of silver ions in the
crystalline ion conductor Ag7P3S11 is analyzed by comparing appropriate
two-time and three-time 109Ag NMR correlation functions. The non-exponentiality
is due to a rate distribution, i.e., dynamic heterogeneities, rather than to an
intrinsic non-exponentiality. Thus, the data give no evidence for the relevance
of correlated back-and-forth jumps on the timescale of the silver relaxation.Comment: 4 pages, 3 figure
Microscopic Theory of Heterogeneity and Non-Exponential Relaxations in Supercooled Liquids
Recent experiments and computer simulations show that supercooled liquids
around the glass transition temperature are "dynamically heterogeneous" [1].
Such heterogeneity is expected from the random first order transition theory of
the glass transition. Using a microscopic approach based on this theory, we
derive a relation between the departure from Debye relaxation as characterized
by the value of a stretched exponential response function , and the fragility of the liquid. The
value is also predicted to depend on temperature and to vanish as the ideal
glass transition is approached at the Kauzmann temperature.Comment: 4 pages including 3 eps figure
Dynamic heterogeneities in the out-of-equilibrium dynamics of simple spherical spin models
The response of spherical two-spin interaction models, the spherical
ferromagnet (s-FM) and the spherical Sherrington-Kirkpatrick (s-SK) model, is
calculated for the protocol of the so-called nonresonant hole burning
experiment (NHB) for temperatures below the respective critical temperatures.
It is shown that it is possible to select dynamic features in the
out-of-equilibrium dynamics of both models, one of the hallmarks of dynamic
heterogeneities. The behavior of the s-SK model and the s-FM in three
dimensions is very similar, showing dynamic heterogeneities in the long time
behavior, i.e. in the aging regime. The appearence of dynamic heterogeneities
in the s-SK model explicitly demonstrates that these are not necessarily
related to {\it spatial} heterogeneities. For the s-FM it is shown that the
nature of the dynamic heterogeneities changes as a function of dimensionality.
With incresing dimension the frequency selectivity of the NHB diminishes and
the dynamics in the mean-field limit of the s-FM model becomes homogeneous.Comment: 16 pages, 8 figure
Multiple-Point and Multiple-Time Correlations Functions in a Hard-Sphere Fluid
A recent mode coupling theory of higher-order correlation functions is tested
on a simple hard-sphere fluid system at intermediate densities. Multi-point and
multi-time correlation functions of the densities of conserved variables are
calculated in the hydrodynamic limit and compared to results obtained from
event-based molecular dynamics simulations. It is demonstrated that the mode
coupling theory results are in excellent agreement with the simulation results
provided that dissipative couplings are included in the vertices appearing in
the theory. In contrast, simplified mode coupling theories in which the
densities obey Gaussian statistics neglect important contributions to both the
multi-point and multi-time correlation functions on all time scales.Comment: Second one in a sequence of two (in the first, the formalism was
developed). 12 pages REVTeX. 5 figures (eps). Submitted to Phys.Rev.
Structural Probe of a Glass Forming Liquid: Generalized Compressibility
We introduce a new quantity to probe the glass transition. This quantity is a
linear generalized compressibility which depends solely on the positions of the
particles. We have performed a molecular dynamics simulation on a glass forming
liquid consisting of a two component mixture of soft spheres in three
dimensions. As the temperature is lowered (or as the density is increased), the
generalized compressibility drops sharply at the glass transition, with the
drop becoming more and more abrupt as the measurement time increases. At our
longest measurement times, the drop occurs approximately at the mode coupling
temperature . The drop in the linear generalized compressibility occurs at
the same temperature as the peak in the specific heat. By examining the
inherent structure energy as a function of temperature, we find that our
results are consistent with the kinetic view of the glass transition in which
the system falls out of equilibrium. We find no size dependence and no evidence
for a second order phase transition though this does not exclude the
possibility of a phase transition below the observed glass transition
temperature. We discuss the relation between the linear generalized
compressibility and the ordinary isothermal compressibility as well as the
static structure factor.Comment: 18 pages, Latex, 26 encapsulated postscript figures, revised paper is
shorter, to appear in Phys. Rev.
Time and length scales in supercooled liquids
We numerically obtain the first quantitative demonstration that development
of spatial correlations of mobility as temperature is lowered is responsible
for the ``decoupling'' of transport properties of supercooled liquids. This
result further demonstrates the necessity of a spatial description of the glass
formation and therefore seriously challenges a number of popular alternative
theoretical descriptions.Comment: 4 pages, 4 figs; improved version: new refs and discussion
Mode-coupling theory for multiple-time correlation functions of tagged particle densities and dynamical filters designed for glassy systems
The theoretical framework for higher-order correlation functions involving
multiple times and multiple points in a classical, many-body system developed
by Van Zon and Schofield [Phys. Rev. E 65, 011106 (2002)] is extended here to
include tagged particle densities. Such densities have found an intriguing
application as proposed measures of dynamical heterogeneities in structural
glasses. The theoretical formalism is based upon projection operator techniques
which are used to isolate the slow time evolution of dynamical variables by
expanding the slowly-evolving component of arbitrary variables in an infinite
basis composed of the products of slow variables of the system. The resulting
formally exact mode-coupling expressions for multiple-point and multiple-time
correlation functions are made tractable by applying the so-called N-ordering
method. This theory is used to derive for moderate densities the leading mode
coupling expressions for indicators of relaxation type and domain relaxation,
which use dynamical filters that lead to multiple-time correlations of a tagged
particle density. The mode coupling expressions for higher order correlation
functions are also succesfully tested against simulations of a hard sphere
fluid at relatively low density.Comment: 15 pages, 2 figure
Growing Correlation Length on Cooling Below the Onset of Caging in a Simulated Glass-Forming Liquid
We present a calculation of a fourth-order, time-dependent density
correlation function that measures higher-order spatiotemporall correlations of
the density of a liquid. From molecular dynamics simulations of a glass-forming
Lennard-Jones liquid, we find that the characteristic length scale of this
function has a maximum as a function of time which increases steadily beyond
the characteristic length of the static pair correlation function in the
temperature range approaching the mode coupling temperature from above
The Shapes of Cooperatively Rearranging Regions in Glass Forming Liquids
The shapes of cooperatively rearranging regions in glassy liquids change from
being compact at low temperatures to fractal or ``stringy'' as the dynamical
crossover temperature from activated to collisional transport is approached
from below. We present a quantitative microscopic treatment of this change of
morphology within the framework of the random first order transition theory of
glasses. We predict a correlation of the ratio of the dynamical crossover
temperature to the laboratory glass transition temperature, and the heat
capacity discontinuity at the glass transition, Delta C_p. The predicted
correlation agrees with experimental results for the 21 materials compiled by
Novikov and Sokolov.Comment: 9 pages, 6 figure
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