State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, People's Republic of China.
J Phys Condens Matter. 2012 Aug 15;24(32):325101, 1-11. doi: 10.1088/0953-8984/24/32/325101. Epub 2012 May 31.
We numerically study dynamics and correlation length scales of a colloidal liquid in both quiescent and sheared conditions to further understand the origin of slow dynamics and dynamic heterogeneity in glass-forming systems. The simulation is performed in a weakly frustrated two-dimensional liquid, where locally preferred order is allowed to develop with increasing density. The four-point density correlations and bond-orientation correlations, which have been frequently used to capture dynamic and static length scales ξ in a quiescent condition, can be readily extended to a system under steady shear in this case. In the absence of shear, we confirmed the previous findings that the dynamic slowing down accompanies the development of dynamic heterogeneity. The dynamic and static length scales increase with α-relaxation time τ(α) as a power law [Formula: see text], with μ > 0. In the presence of shear, both viscosity and τ(α) have power-law dependences on shear rate in the marked shear-thinning regime. However, the dependence of correlation lengths cannot be described by power laws in the same regime. Furthermore, the relation [Formula: see text] between length scales and dynamics holds for not too strong shear where thermal fluctuations and external forces are both important in determining the properties of dense liquids. Thus, our results demonstrate a link between slow dynamics and structure in glass-forming liquids even under nonequilibrium conditions.
我们通过数值模拟研究了静止和剪切条件下胶体液体的动力学和相关长度尺度,以进一步了解玻璃形成体系中慢动力学和动态异质性的起源。该模拟在弱受挫二维液体中进行,局部优先顺序随着密度的增加而发展。四点密度相关函数和键取向相关函数常用于在静止条件下捕捉动态和静态长度尺度 ξ,在这种情况下,它们可以很容易地扩展到稳态剪切系统。在没有剪切的情况下,我们证实了先前的发现,即动态减速伴随着动态异质性的发展。动态和静态长度尺度随 α 弛豫时间 τ(α)呈幂律关系 [公式:见文本],其中 μ > 0。在剪切存在的情况下,在明显的剪切稀化区域,粘度和 τ(α) 对剪切率都有幂律依赖性。然而,在相同的区域,相关长度的依赖性不能用幂律来描述。此外,在决定稠密液体性质时,热涨落和外力都很重要的情况下,长度尺度和动力学之间的关系 [公式:见文本] 适用于不太强的剪切。因此,我们的结果表明,即使在非平衡条件下,玻璃形成液体的慢动力学和结构之间也存在联系。