Institut für Theoretische Physik, Universität Innsbruck, Technikerstraße 21A, A-6020 Innsbruck, Austria.
Soft Matter. 2017 Sep 20;13(36):6167-6177. doi: 10.1039/c7sm00905d.
Within a recently developed mode-coupling theory for fluids confined to a slit we elaborate numerical results for the long-time limits of suitably generalized intermediate scattering functions. The theory requires as input the density profile perpendicular to the plates, which we obtain from density functional theory within the fundamental-measure framework, as well as symmetry-adapted static structure factors, which can be calculated relying on the inhomogeneous Percus-Yevick closure. Our calculations for the nonergodicity parameters for both the collective as well as for the self motion are in qualitative agreement with our extensive event-driven molecular dynamics simulations for the intermediate scattering functions for slightly polydisperse hard-sphere systems at high packing fraction. We show that the variation of the nonergodicity parameters as a function of the wavenumber correlates with the in-plane static structure factors, while subtle effects become apparent in the structure factors and relaxation times of higher mode indices. A criterion to predict the multiple reentrant from the variation of the in-plane static structure is presented.
在最近发展的用于狭缝中受限流体的模式耦合理论中，我们详细阐述了适用于广义中间散射函数的长时间极限的数值结果。该理论需要输入垂直于板的密度分布，我们从基本测度框架中的密度泛函理论中获得密度分布，以及对称自适应静态结构因子，我们可以依靠非均匀 Percus-Yevick 闭合来计算这些结构因子。我们对集体和自运动的非遍历参数的计算与我们对中间散射函数的广泛事件驱动分子动力学模拟结果定性一致，这些模拟是针对高填充分数下具有轻微多分散硬球系统的。我们表明，非遍历参数随波数的变化与面内静态结构因子相关，而在更高模式指数的结构因子和弛豫时间中出现了细微的影响。提出了一个根据面内静态结构变化来预测多重再进入的判据。
