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玻璃形成液体动力学中的空间相关性:其温度依赖性的实验测定

Spatial correlations in the dynamics of glassforming liquids: experimental determination of their temperature dependence.

作者信息

Dalle-Ferrier C, Thibierge C, Alba-Simionesco C, Berthier L, Biroli G, Bouchaud J-P, Ladieu F, L'Hôte D, Tarjus G

机构信息

Laboratoire de Chimie Physique, UMR 8000, Université Paris Sud and CNRS, Bâtiment 349, 91405 Orsay, France.

出版信息

Phys Rev E Stat Nonlin Soft Matter Phys. 2007 Oct;76(4 Pt 1):041510. doi: 10.1103/PhysRevE.76.041510. Epub 2007 Oct 29.

Abstract

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.

摘要

我们使用最近引入的三点动态磁化率来对过冷液体结构弛豫过程中动态相关的分子数(N_{corr})的温度演化进行实验测定。我们首先详细讨论三点函数的物理内涵,这些函数将平均双时动力学对外部控制参数(如温度或密度)的敏感性联系起来,以及它们与与动力学非均匀性相关的更标准的四点动态磁化率的联系。然后我们证明这些函数可以通过实验高精度地测定。我们收集现有数据,以获得大量过冷液体在从玻璃化转变到慢动力学开始的广泛弛豫时间尺度范围内(N_{corr})的温度依赖性。我们发现,当接近玻璃化转变时,(N_{corr})会系统性地增加。在接近玻璃化转变时,它以适度的方式增加,这与基于活化的玻璃形成材料动力学图像一致。对于较高温度,似乎存在一个(N_{corr})表现为弛豫时间幂律的区域。最后,我们发现对密度的动态响应虽然小于对温度的动态响应,但表现相似,这与理论预期一致。

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