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高度尺寸非对称二元硬磁盘液体的结构、压缩因子和动力学。

Structure, compressibility factor, and dynamics of highly size-asymmetric binary hard-disk liquids.

机构信息

State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, People's Republic of China.

出版信息

J Chem Phys. 2012 Sep 14;137(10):104509. doi: 10.1063/1.4751546.

Abstract

By using event-driven molecular dynamics simulation, we investigate effects of varying the area fraction of the smaller component on structure, compressibility factor, and dynamics of the highly size-asymmetric binary hard-disk liquids. We find that the static pair correlations of the large disks are only weakly perturbed by adding small disks. The higher-order static correlations of the large disks, by contrast, can be strongly affected. Accordingly, the static correlation length deduced from the bond-orientation correlation functions first decreases significantly and then tends to reach a plateau as the area fraction of the small disks increases. The compressibility factor of the system first decreases and then increases upon increasing the area fraction of the small disks and separating different contributions to it allows to rationalize this non-monotonic phenomenon. Furthermore, adding small disks can influence dynamics of the system in quantitative and qualitative ways. For the large disks, the structural relaxation time increases monotonically with increasing the area fraction of the small disks at low and moderate area fractions of the large disks. In particular, "reentrant" behavior appears at sufficiently high area fractions of the large disks, strongly resembling the reentrant glass transition in short-ranged attractive colloids and the inverted glass transition in binary hard spheres with large size disparity. By tuning the area fraction of the small disks, relaxation process for the small disks shows concave-to-convex crossover and logarithmic decay behavior, as found in other binary mixtures with large size disparity. Moreover, diffusion of both species is suppressed by adding small disks. Long-time diffusion for the small disks shows power-law-like behavior at sufficiently high area fractions of the small disks, which implies precursors of a glass transition for the large disks and a localization transition for the small disks. Therefore, our results demonstrate the generic dynamic features in highly size-asymmetric binary mixtures.

摘要

利用事件驱动的分子动力学模拟,我们研究了较小成分的面积分数变化对高度尺寸不对称二元硬磁盘液体的结构、压缩因子和动力学的影响。我们发现,加入小磁盘仅会对大磁盘的静态对相关函数产生微弱的干扰。相比之下,大磁盘的高阶静态相关函数可能会受到强烈影响。因此,从键取向相关函数推导出的静态相关长度首先显著减小,然后随着小磁盘面积分数的增加趋于达到一个平台。随着小磁盘面积分数的增加,系统的压缩因子先减小后增大,通过分离对其的不同贡献,可以合理化这种非单调现象。此外,添加小磁盘可以在定量和定性方面影响系统的动力学。对于大磁盘,在低和中等大磁盘面积分数下,结构弛豫时间随着小磁盘面积分数的增加而单调增加。特别是,在足够大的大磁盘面积分数下,会出现“重入”行为,这与短程吸引胶体中的重入玻璃转变和具有大尺寸差异的二元硬球中的反向玻璃转变强烈相似。通过调整小磁盘的面积分数,小磁盘的弛豫过程表现出凹向凸的交叉和对数衰减行为,如在其他具有大尺寸差异的二元混合物中发现的那样。此外,添加小磁盘会抑制两种物质的扩散。在足够大的小磁盘面积分数下,小磁盘的长时间扩散表现出幂律行为,这意味着大磁盘的玻璃化转变前体和小磁盘的局部化转变前体。因此,我们的结果展示了高度尺寸不对称二元混合物中的通用动力学特征。

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