Charbonneau P, Ikeda A, van Meel J A, Miyazaki K
Department of Chemistry, Duke University, Durham, North Carolina 27708, USA.
Phys Rev E Stat Nonlin Soft Matter Phys. 2010 Apr;81(4 Pt 1):040501. doi: 10.1103/PhysRevE.81.040501. Epub 2010 Apr 14.
There exists a variety of theories of the glass transition and many more numerical models. But because the models need built-in complexity to prevent crystallization, comparisons with theory can be difficult. We study the dynamics of a deeply supersaturated monodisperse four-dimensional (4D) hard-sphere fluid, which has no such complexity, but whose strong intrinsic geometrical frustration inhibits crystallization, even when deeply supersaturated. As an application, we compare its behavior to the mode-coupling theory (MCT) of glass formation. We find MCT to describe this system better than any other structural glass formers in lower dimensions. The reduction in dynamical heterogeneity in 4D suggested by a milder violation of the Stokes-Einstein relation could explain the agreement. These results are consistent with a mean-field scenario of the glass transition.
存在多种玻璃化转变理论以及更多的数值模型。但由于这些模型需要内在的复杂性来防止结晶,所以与理论进行比较可能会很困难。我们研究了一种深度过饱和的单分散四维(4D)硬球流体的动力学,这种流体没有上述复杂性,但其强烈的内在几何挫折抑制了结晶,即使在深度过饱和时也是如此。作为一个应用,我们将其行为与玻璃形成的模式耦合理论(MCT)进行了比较。我们发现MCT对该系统的描述比低维中的任何其他结构玻璃形成体都要好。由对斯托克斯 - 爱因斯坦关系的较温和违反所暗示的4D中动力学非均匀性的降低可以解释这种一致性。这些结果与玻璃化转变的平均场情景一致。