Spatial correlations in the dynamics of glassforming liquids: experimental determination of their temperature dependence.
We use recently introduced three-point dynamic susceptibilities to obtain an experimental determination of the temperature evolution of the number of molecules Ncorr that are dynamically correlated during the structural relaxation of supercooled liquids. We first discuss in detail the physical content of three-point functions that relate the sensitivity of the averaged two-time dynamics to external control parameters (such as temperature or density), as well as their connection to the more standard four-point dynamic susceptibility associated with dynamical heterogeneities. We then demonstrate that these functions can be experimentally determined with good precision. We gather available data to obtain the temperature dependence of Ncorr for a large number of supercooled liquids over a wide range of relaxation time scales from the glass transition up to the onset of slow dynamics. We find that Ncorr systematically grows when approaching the glass transition. It does so in a modest manner close to the glass transition, which is consistent with an activation-based picture of the dynamics in glassforming materials. For higher temperatures, there appears to be a regime where Ncorr behaves as a power-law of the relaxation time. Finally, we find that the dynamic response to density, while being smaller than the dynamic response to temperature, behaves similarly, in agreement with theoretical expectations.
Dalle-Ferrier
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C
Laboratoire de Chimie Physique, UMR 8000, Université Paris Sud and CNRS, Bâtiment 349, 91405 Orsay, France.
Thibierge
C
C
Alba-Simionesco
C
C
Berthier
L
L
Biroli
G
G
Bouchaud
J-P
JP
Ladieu
F
F
L'Hôte
D
D
Tarjus
G
G