101 research outputs found
How do the properties of a glass depend on the cooling rate? A computer simulation study of a Lennard-Jones system
Using molecular dynamics computer simulations we investigate how the glass
transition and the properties of the resulting glass depend on the cooling rate
with which the sample has been quenched. This is done by studying a two
component Lennard-Jones system which is coupled to a heat bath whose
temperature is decreased from a high temperature, where the system is a liquid,
to zero temperature, where the system is a glass. The temperature of the
heat bath is decreased linearly in time, i.e. , where
is the cooling rate. In accordance with simple theoretical arguments
and with experimental observations we find that the glass transition, as
observed in the specific heat and the thermal expansion coefficient, becomes
sharper when is decreased. A decrease of the cooling rate also leads
to a decrease of the glass transition temperature and we show that the
dependence of on can be rationalized by assuming that the
temperature dependence of the relaxation times of the system is given by either
a Vogel-Fulcher law or a power-law. By investigating the structural properties
of the glass, such as the radial distribution functions, the coordination
numbers and the angles between three neighbor-sharing particles, we show how
the local order of the glass increases with decreasing cooling rate. The
enthalpy and the density of the glass decrease and increase, respectively, with
decreasing . By investigating the dependence of clusters of
nearest neighbors, we show how these observations can be understood from a
microscopic point of view. We also show that the spectrum of the glass, as
computed from the dynamical matrix, shows a shift towards higher frequencies
when is decreased. All these effects show that there is a significantComment: 20 pages of RevTex, Figures available upon request from W. Ko
Temperature in nonequilibrium systems with conserved energy
We study a class of nonequilibrium lattice models which describe local
redistributions of a globally conserved energy. A particular subclass can be
solved analytically, allowing to define a temperature T_{th} along the same
lines as in the equilibrium microcanonical ensemble. The
fluctuation-dissipation relation is explicitely found to be linear, but its
slope differs from the inverse temperature T_{th}^{-1}. A numerical
renormalization group procedure suggests that, at a coarse-grained level, all
models behave similarly, leading to a two-parameter description of their
macroscopic properties.Comment: 4 pages, 1 figure, final versio
Kovacs effects in an aging molecular liquid
We study by means of molecular dynamics simulations the aging behavior of a
molecular model of ortho-terphenyl. We find evidence of a a non-monotonic
evolution of the volume during an isothermal-isobaric equilibration process, a
phenomenon known in polymeric systems as Kovacs effect. We characterize this
phenomenology in terms of landscape properties, providing evidence that, far
from equilibrium, the system explores region of the potential energy landscape
distinct from the one explored in thermal equilibrium. We discuss the relevance
of our findings for the present understanding of the thermodynamics of the
glass state.Comment: RevTeX 4, 4 pages, 5 eps figure
Thermodynamics of the glassy state: effective temperature as an additional system parameter
A system is glassy when the observation time is much smaller than the
equilibration time. A unifying thermodynamic picture of the glassy state is
presented. Slow configurational modes are in quasi-equilibrium at an effective
temperature. It enters thermodynamic relations with the configurational entropy
as conjugate variable. Slow fluctuations contribute to susceptibilities via
quasi-equilibrium relations, while there is also a configurational term.
Fluctuation-dissipation relations also involve the effective temperature.
Fluctuations in the energy are non-universal, however. The picture is supported
by analytically solving the dynamics of a toy model.Comment: 5 pages, REVTEX. Phys. Rev. Lett, to appea
Thermodynamics of black holes: an analogy with glasses
The present equilibrium formulation of thermodynamics for black holes has
several drawbacks, such as assuming the same temperature for black hole and
heat bath. Recently the author formulated non-equilibrium thermodynamics for
glassy systems. This approach is applied to black holes, with the cosmic
background temperature being the bath temperature, and the Hawking temperature
the internal temperature. Both Hawking evaporation and absorption of background
radiation are taken into account.
It is argued that black holes did not form in the very early universe.Comment: 4 pages revtex; submitted to Phys. Rev. Let
The Glass Transition Temperature of Water: A Simulation Study
We report a computer simulation study of the glass transition for water. To
mimic the difference between standard and hyperquenched glass, we generate
glassy configurations with different cooling rates and calculate the
dependence of the specific heat on heating. The absence of crystallization
phenomena allows us, for properly annealed samples, to detect in the specific
heat the simultaneous presence of a weak pre-peak (``shadow transition''), and
an intense glass transition peak at higher temperature.
We discuss the implications for the currently debated value of the glass
transition temperature of water. We also compare our simulation results with
the Tool-Narayanaswamy-Moynihan phenomenological model.Comment: submitted to Phys. Re
Thermodynamic picture of the glassy state
A picture for thermodynamics of the glassy state is introduced. It assumes
that one extra parameter, the effective temperature, is needed to describe the
glassy state. This explains the classical paradoxes concerning the Ehrenfest
relations and the Prigogine-Defay ratio. As a second part, the approach
connects the response of macroscopic observables to a field change with their
temporal fluctuations, and with the fluctuation-dissipation relation, in a
generalized non-equilibrium way.Comment: Proceedings of the Conference "Unifying Concepts in Glass Physics",
ICTP, Trieste, 15 - 18 September 199
Minimal model for beta relaxation in viscous liquids
Contrasts between beta relaxation in equilibrium viscous liquids and glasses
are rationalized in terms of a double-well potential model with
structure-dependent asymmetry, assuming structure is described by a single
order parameter. The model is tested for tripropylene glycol where it accounts
for the hysteresis of the dielectric beta loss peak frequency and magnitude
during cooling and reheating through the glass transition.Comment: Phys. Rev. Lett. (in press
Observation of Fluctuation-Dissipation-Theorem Violations in a Structural Glass
The fluctuation-dissipation theorem (FDT), connecting dielectric
susceptibility and polarization noise was studied in glycerol below its glass
transition temperature Tg. Weak FDT violations were observed after a quench
from just above to just below Tg, for frequencies above the alpha peak.
Violations persisted up to 10^5 times the thermal equilibration time of the
configurational degrees of freedom under study, but comparable to the average
relaxation time of the material. These results suggest that excess energy flows
from slower to faster relaxing modes.Comment: Improved discussion; final version to appear in Phys. Rev. Lett. 4
pages, 5 PS figures, RevTe
Computer Simulations of Supercooled Liquids and Glasses
After a brief introduction to the dynamics of supercooled liquids, we discuss
some of the advantages and drawbacks of computer simulations of such systems.
Subsequently we present the results of computer simulations in which the
dynamics of a fragile glass former, a binary Lennard-Jones system, is compared
to the one of a strong glass former, SiO_2. This comparison gives evidence that
the reason for the different temperature dependence of these two types of glass
formers lies in the transport mechanism for the particles in the vicinity of
T_c, the critical temperature of mode-coupling theory. Whereas the one of the
fragile glass former is described very well by the ideal version of
mode-coupling theory, the one for the strong glass former is dominated by
activated processes. In the last part of the article we review some simulations
of glass formers in which the dynamics below the glass transition temperature
was investigated. We show that such simulations might help to establish a
connection between systems with self generated disorder (e.g. structural
glasses) and quenched disorder (e.g. spin glasses).Comment: 37 pages of Latex, 11 figures, to appear as a Topical Review article
in J. Phys.: Condens. Matte
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