121 research outputs found
Non-monotonic temperature evolution of dynamic correlations in glass-forming liquids
The viscosity of glass-forming liquids increases by many orders of magnitude
if their temperature is lowered by a mere factor of 2-3 [1,2]. Recent studies
suggest that this widespread phenomenon is accompanied by spatially
heterogeneous dynamics [3,4], and a growing dynamic correlation length
quantifying the extent of correlated particle motion [5-7]. Here we use a novel
numerical method to detect and quantify spatial correlations which reveal a
surprising non-monotonic temperature evolution of spatial dynamical
correlations, accompanied by a second length scale that grows monotonically and
has a very different nature. Our results directly unveil a dramatic qualitative
change in atomic motions near the mode-coupling crossover temperature [8] which
involves no fitting or indirect theoretical interpretation. Our results impose
severe new constraints on the theoretical description of the glass transition,
and open several research perspectives, in particular for experiments, to
confirm and quantify our observations in real materials.Comment: 7 page
Irreversible reorganization in a supercooled liquid originates from localised soft modes
The transition of a fluid to a rigid glass upon cooling is a common route of
transformation from liquid to solid that embodies the most poorly understood
features of both phases1,2,3. From the liquid perspective, the puzzle is to
understand stress relaxation in the disordered state. From the perspective of
solids, the challenge is to extend our description of structure and its
mechanical consequences to materials without long range order. Using computer
simulations, we show that the localized low frequency normal modes of a
configuration in a supercooled liquid are causally correlated to the
irreversible structural reorganization of the particles within that
configuration. We also demonstrate that the spatial distribution of these soft
local modes can persist in spite of significant particle reorganization. The
consequence of these two results is that it is now feasible to construct a
theory of relaxation length scales in glass-forming liquids without recourse to
dynamics and to explicitly relate molecular properties to their collective
relaxation.Comment: Published online: 20 July 2008 | doi:10.1038/nphys1025 Available from
http://www.nature.com/nphys/journal/v4/n9/abs/nphys1025.htm
Unexpected drop of dynamical heterogeneities in colloidal suspensions approaching the jamming transition
As the glass (in molecular fluids\cite{Donth}) or the jamming (in colloids
and grains\cite{LiuNature1998}) transitions are approached, the dynamics slow
down dramatically with no marked structural changes. Dynamical heterogeneity
(DH) plays a crucial role: structural relaxation occurs through correlated
rearrangements of particle ``blobs'' of size
\cite{WeeksScience2000,DauchotPRL2005,Glotzer,Ediger}. On approaching
these transitions, grows in glass-formers\cite{Glotzer,Ediger},
colloids\cite{WeeksScience2000,BerthierScience2005}, and driven granular
materials\cite{KeysNaturePhys2007} alike, strengthening the analogies between
the glass and the jamming transitions. However, little is known yet on the
behavior of DH very close to dynamical arrest. Here, we measure in colloids the
maximum of a ``dynamical susceptibility'', , whose growth is usually
associated to that of \cite{LacevicPRE}. initially increases with
volume fraction , as in\cite{KeysNaturePhys2007}, but strikingly drops
dramatically very close to jamming. We show that this unexpected behavior
results from the competition between the growth of and the reduced
particle displacements associated with rearrangements in very dense
suspensions, unveiling a richer-than-expected scenario.Comment: 1st version originally submitted to Nature Physics. See the Nature
Physics website fro the final, published versio
Thermodynamic signature of growing amorphous order in glass-forming liquids
Although several theories relate the steep slowdown of glass formers to
increasing spatial correlations of some sort, standard static correlation
functions show no evidence for this. We present results that reveal for the
first time a qualitative thermodynamic difference between the high temperature
and deeply supercooled equilibrium glass-forming liquid: the influence of
boundary conditions propagates into the bulk over larger and larger
lengthscales upon cooling, and, as this static correlation length grows, the
influence decays nonexponentially. Increasingly long-range susceptibility to
boundary conditions is expected within the random firt-order theory (RFOT) of
the glass transition, but a quantitative account of our numerical results
requires a generalization of RFOT where the surface tension between states
fluctuates
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
Holographic Vitrification
We establish the existence of stable and metastable stationary black hole
bound states at finite temperature and chemical potentials in global and planar
four-dimensional asymptotically anti-de Sitter space. We determine a number of
features of their holographic duals and argue they represent structural
glasses. We map out their thermodynamic landscape in the probe approximation,
and show their relaxation dynamics exhibits logarithmic aging, with aging rates
determined by the distribution of barriers.Comment: 100 pages, 25 figure
Rejuvenation of metallic glasses by non-affine thermal strain.
When a spatially uniform temperature change is imposed on a solid with more than one phase, or on a polycrystal of a single, non-cubic phase (showing anisotropic expansion-contraction), the resulting thermal strain is inhomogeneous (non-affine). Thermal cycling induces internal stresses, leading to structural and property changes that are usually deleterious. Glasses are the solids that form on cooling a liquid if crystallization is avoided--they might be considered the ultimate, uniform solids, without the microstructural features and defects associated with polycrystals. Here we explore the effects of cryogenic thermal cycling on glasses, specifically metallic glasses. We show that, contrary to the null effect expected from uniformity, thermal cycling induces rejuvenation, reaching less relaxed states of higher energy. We interpret these findings in the context that the dynamics in liquids become heterogeneous on cooling towards the glass transition, and that there may be consequent heterogeneities in the resulting glasses. For example, the vibrational dynamics of glassy silica at long wavelengths are those of an elastic continuum, but at wavelengths less than approximately three nanometres the vibrational dynamics are similar to those of a polycrystal with anisotropic grains. Thermal cycling of metallic glasses is easily applied, and gives improvements in compressive plasticity. The fact that such effects can be achieved is attributed to intrinsic non-uniformity of the glass structure, giving a non-uniform coefficient of thermal expansion. While metallic glasses may be particularly suitable for thermal cycling, the non-affine nature of strains in glasses in general deserves further study, whether they are induced by applied stresses or by temperature change.This research was supported by the World Premier International Research Center Initiative (WPI), MEXT, Japan, by NSF China and MOST 973 China, and by the Engineering and the Engineering and Physical Sciences Research Council, UK (Materials World Network project). Y.H.S. acknowledges support from a China Scholarship Council (CSC) scholarship.This is the author accepted manuscript. The final version is available from Nature Publishing Group via http://dx.doi.org/10.1038/nature1467
Glass transition with decreasing correlation length during cooling of Fe50Co50 superlattice and strong liquids
The glass transition GT is usually thought of as a structural arrest that
occurs during the cooling of a liquid, or sometimes a plastic crystal, trapping
a metastable state of the system before it can recrystallize to stabler forms1.
This phenomenon occurs in liquids of all classes, most recently in bulk
metallic glassformers2. Much theoretical interest has been generated by the
dynamical heterogeneity observed in cooling of fragile liquids3, 4, and many
have suggested that the slow-down is caused by a related increasing correlation
length 5-9. Here we report both kinetics and thermodynamics of arrest in a
system that disorders while in its ground state, exhibits a large !Cp on arrest
(!Cp = Cp,mobile - Cp,arrested), yet clearly is characterized by a correlation
length that is decreasing as GT is approached from above. We show that GT
kinetics in our system, the disordering superlattice Fe50Co50, satisfy the
kinetic criterion for ideally 'strong' glassformers10, and since !Cp behavior
through Tg also correlates10, we propose that very strong liquidsand very
fragile liquids exist on opposite flanks of an order-disorder transition - one
that is already known for model systems
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