Berthier L, Tarjus G
Laboratoire Charles Coulomb, CNRS-UMR 5221, Université Montpellier 2, Place Eugène Bataillon, 34095 Montpellier Cedex, France.
Eur Phys J E Soft Matter. 2011 Sep;34(9):96. doi: 10.1140/epje/i2011-11096-5. Epub 2011 Sep 23.
We assess the validity of "microscopic" approaches of glass-forming liquids based on the sole knowledge of the static pair density correlations. To do so, we apply them to a benchmark provided by two liquid models that share very similar static pair density correlation functions while displaying distinct temperature evolutions of their relaxation times. We find that the approaches are unsuccessful in describing the difference in the dynamical behavior of the two models. Our study is not exhaustive, and we have not tested the effect of adding corrections by including, for instance, three-body density correlations. Yet, our results appear strong enough to challenge the claim that the slowdown of relaxation in glass-forming liquids, for which it is well established that the changes of the static structure factor with temperature are small, can be explained by "microscopic" approaches only requiring the static pair density correlations as nontrivial input.
我们基于静态对密度关联的唯一知识来评估玻璃形成液体“微观”方法的有效性。为此,我们将它们应用于由两个液体模型提供的基准,这两个模型具有非常相似的静态对密度关联函数,同时其弛豫时间呈现出不同的温度演变。我们发现这些方法在描述两个模型动力学行为的差异方面并不成功。我们的研究并不详尽,并且我们尚未测试通过纳入例如三体密度关联来添加修正的效果。然而,我们的结果似乎足够有力,足以挑战这样一种说法,即对于玻璃形成液体中弛豫的减慢(众所周知,其静态结构因子随温度的变化很小),可以仅通过将静态对密度关联作为重要输入的“微观”方法来解释。