92 research outputs found
Thermodynamic scaling of diffusion in supercooled Lennard-Jones liquids
The manner in which the intermolecular potential u(r) governs structural
relaxation in liquids is a long standing problem in condensed matter physics.
Herein we show that diffusion coefficients for simulated Lennard-Jones m-6
liquids (8<m<36) in normal and moderately supercooled states are a unique
function of the variable rho^g/T, where rho is density and T is temperature.
The scaling exponent g is a material specific constant whose magnitude is
related to the steepness of the repulsive part of u(r), evaluated around the
distance of closest approach between particles probed in the supercooled
regime. Approximations of u(r) in terms of inverse power laws are also
discussed.Comment: 4 pages, 3 figure
Density scaling in viscous liquids: From relaxation times to four-point susceptibilities
We present numerical calculations of a four-point dynamic susceptibility,
chi_4(t), for the Kob-Andersen Lennard-Jones mixture as a function of
temperature T and density rho. Over a relevant range of T and rho, the full
t-dependence of chi_4(t) and thus the maximum in chi_4(t), which is
proportional to the dynamic correlation volume, are invariant for state points
for which the scaling variable rho^gamma/T is constant. The value of the
material constant gamma is the same as that which superposes the relaxation
time, tau, of the system versus rho^gamma/T. Thus, the dynamic correlation
volume is directly related to tau for any thermodynamic condition in the regime
where density scaling holds. Finally, we examine the conditions under which the
density scaling properties are related to the existence of strong correlations
between pressure and energy fluctuations.Comment: 5 pages, 4 figures, updated reference
Dynamics and energy landscape in a tetrahedral network glass-former: Direct comparison with models of fragile liquids
We report Molecular Dynamics simulations for a new model of tetrahedral
network glass-former, based on short-range, spherical potentials. Despite the
simplicity of the forcefield employed, our model reproduces some essential
physical properties of silica, an archetypal network-forming material.
Structural and dynamical properties, including dynamic heterogeneities and the
nature of local rearrangements, are investigated in detail and a direct
comparison with models of close-packed, fragile glass-formers is performed. The
outcome of this comparison is rationalized in terms of the properties of the
Potential Energy Surface, focusing on the unstable modes of the stationary
points. Our results indicate that the weak degree of dynamic heterogeneity
observed in network glass-formers may be attributed to an excess of localized
unstable modes, associated to elementary dynamical events such as bond breaking
and reformation. On the contrary, the more fragile Lennard-Jones mixtures are
characterized by a larger fraction of extended unstable modes, which lead to a
more cooperative and heterogeneous dynamics.Comment: 26 pages, 18 figures, added links to animations, corrected typos in
sec.
Ultrafast Dynamics of Vibrational Symmetry Breaking in a Charge-ordered Nickelate
The ability to probe symmetry breaking transitions on their natural time
scales is one of the key challenges in nonequilibrium physics. Stripe ordering
represents an intriguing type of broken symmetry, where complex interactions
result in atomic-scale lines of charge and spin density. Although phonon
anomalies and periodic distortions attest the importance of electron-phonon
coupling in the formation of stripe phases, a direct time-domain view of
vibrational symmetry breaking is lacking. We report experiments that track the
transient multi-THz response of the model stripe compound
LaSrNiO, yielding novel insight into its electronic and
structural dynamics following an ultrafast optical quench. We find that
although electronic carriers are immediately delocalized, the crystal symmetry
remains initially frozen - as witnessed by time-delayed suppression of
zone-folded Ni-O bending modes acting as a fingerprint of lattice symmetry.
Longitudinal and transverse vibrations react with different speeds, indicating
a strong directionality and an important role of polar interactions. The hidden
complexity of electronic and structural coupling during stripe melting and
formation, captured here within a single terahertz spectrum, opens new paths to
understanding symmetry breaking dynamics in solids.Comment: 21 pages, 4 figures; updated version with journal re
Are there localized saddles behind the heterogeneous dynamics of supercooled liquids?
We numerically study the interplay between heterogeneous dynamics and
properties of negatively curved regions of the potential energy surface in a
model glassy system. We find that the unstable modes of saddles and
quasi-saddles undergo a localization transition close to the Mode-Coupling
critical temperature. We also find evidence of a positive spatial correlation
between clusters of particles having large displacements in the unstable modes
and dynamical heterogeneities.Comment: 7 pages, 3 figures, submitted to Europhys. Let
Heterogeneous Dynamics, Marginal Stability and Soft Modes in Hard Sphere Glasses
In a recent publication we established an analogy between the free energy of
a hard sphere system and the energy of an elastic network [1]. This result
enables one to study the free energy landscape of hard spheres, in particular
to define normal modes. In this Letter we use these tools to analyze the
activated transitions between meta-bassins, both in the aging regime deep in
the glass phase and near the glass transition. We observe numerically that
structural relaxation occurs mostly along a very small number of
nearly-unstable extended modes. This number decays for denser packing and is
significantly lowered as the system undergoes the glass transition. This
observation supports that structural relaxation and marginal modes share common
properties. In particular theoretical results [2, 3] show that these modes
extend at least on some length scale where
corresponds to the maximum packing fraction, i.e. the jamming
transition. This prediction is consistent with very recent numerical
observations of sheared systems near the jamming threshold [4], where a similar
exponent is found, and with the commonly observed growth of the rearranging
regions with compression near the glass transition.Comment: 6 pages, improved versio
Dynamics in binary cluster crystals
As a result of the application of coarse-graining procedures to describe
complex fluids, the study of systems consisting of particles interacting
through bounded, repulsive pair potentials has become of increasing interest in
the last years. A well known example is the so-called Generalized Exponential
Model (GEM-), for which the interaction between particles is described by
the potential . Interactions with
lead to the formation of a novel phase of soft matter consisting of cluster
crystals. Recent studies on the phase behavior of binary mixtures of GEM-
particles have provided evidence for the formation of novel kinds of alloys,
depending on the cross interactions between the two species. This work aims to
study the dynamic behavior of such binary mixtures by means of extensive
molecular dynamics simulations, and in particular to investigate the effect of
the addition of non-clustering particles on the dynamic scenario of
one-component cluster crystals. Analogies and differences with the
one-component case are revealed and discussed by analyzing self- and collective
dynamic correlators.Comment: 17 pages, 8 figures, submitted to JSTA
Strongly correlating liquids and their isomorphs
This paper summarizes the properties of strongly correlating liquids, i.e.,
liquids with strong correlations between virial and potential energy
equilibrium fluctuations at constant volume. We proceed to focus on the
experimental predictions for strongly correlating glass-forming liquids. These
predictions include i) density scaling, ii) isochronal superposition, iii) that
there is a single function from which all frequency-dependent viscoelastic
response functions may be calculated, iv) that strongly correlating liquids are
approximately single-parameter liquids with close to unity Prigogine-Defay
ratio, and v) that the fictive temperature initially decreases for an isobaric
temperature up jump. The "isomorph filter", which allows one to test for
universality of theories for the non-Arrhenius temperature dependence of the
relaxation time, is also briefly discussed
Isomorphs in model molecular liquids
Isomorphs are curves in the phase diagram along which a number of static and
dynamic quantities are invariant in reduced units. A liquid has good isomorphs
if and only if it is strongly correlating, i.e., the equilibrium
virial/potential energy fluctuations are more than 90% correlated in the NVT
ensemble. This paper generalizes isomorphs to liquids composed of rigid
molecules and study the isomorphs of two systems of small rigid molecules, the
asymmetric dumbbell model and the Lewis-Wahnstrom OTP model. In particular, for
both systems we find that the isochoric heat capacity, the excess entropy, the
reduced molecular center-of-mass self part of the intermediate scattering
function, the reduced molecular center-of-mass radial distribution function to
a good approximation are invariant along an isomorph. In agreement with theory,
we also find that an instantaneous change of temperature and density from an
equilibrated state point to another isomorphic state point leads to no
relaxation. The isomorphs of the Lewis-Wahnstrom OTP model were found to be
more approximative than those of the asymmetric dumbbell model, which is
consistent with the OTP model being less strongly correlating. For both models
we find "master isomorphs", i.e., isomorphs have identical shape in the
virial/potential energy phase diagram.Comment: 20 page
Disentangling the electronic and phononic glue in a high-Tc superconductor
Unveiling the nature of the bosonic excitations that mediate the formation of
Cooper pairs is a key issue for understanding unconventional superconductivity.
A fundamen- tal step toward this goal would be to identify the relative weight
of the electronic and phononic contributions to the overall frequency (\Omega)
dependent bosonic function, \Pi(\Omega). We perform optical spectroscopy on
Bi2212 crystals with simultaneous time- and frequency-resolution; this
technique allows us to disentangle the electronic and phononic contributions by
their different temporal evolution. The strength of the interaction
({\lambda}~1.1) with the electronic excitations and their spectral distribution
fully account for the high critical temperature of the superconducting phase
transition.Comment: 9 pages, 4 figure
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