论文标题

通过三重相关函数研究的液体和玻璃状态中简单谐波抑制系统的结构

Structure of the simple harmonic-repulsive system in liquid and glassy states studied by the triple correlation function

论文作者

Levashov, V. A., Ryltsev, R. E., Chtchelkatchev, N. M.

论文摘要

有效描述液体的结构,尤其是在过冷时液体发生的结构变化仍然是一个挑战。在这种情况下,由软颗粒组成的系统特别有趣,因为它们通常表现出非平凡的局部订单,这些命令不允许引入最近邻居外壳的概念。因此,用于软粒子系统的某些方法的使用是为原子液体的结构分析而开发的。在这里,我们报告了使用三重相关函数(TCF)(即不依赖最近邻居概念的方法)对3D中简单谐波驱动液体结构进行的研究。在降压下考虑液体($ p = 1.8 $),在该压力下表现出显着的稳定性,以防止冷却时结晶。证明TCF允许解决结构中的方向相关性的开发,这些相关性不允许从键 - 定向阶参数参数的研究中得出明确的结论。我们的结果表明,如果通过TCF中峰的高度测量的定向相关性,在冷却时会显着增加。柯克伍德的叠加近似无法正确捕获定向排序的这种升高。 TCF中峰形状的详细考虑表明,方向排序与系统动力学的放缓之间存在联系。我们的发现支持这样的观点:液体中定向相关性的发展可能在液体的动力学中起重要作用,并且对配对分布函数的考虑可能不足以理解液体对超冷时液体发生的所有结构变化。

An efficient description of the structures of liquids and, in particular, the structural changes that happen with liquids on supercooling remains to be a challenge. The systems composed of soft particles are especially interesting in this context because they often demonstrate non-trivial local orders that do not allow to introduce the concept of the nearest-neighbor shell. For this reason, the use of some methods, developed for the structure analysis of atomic liquids, is questionable for the soft-particle systems. Here we report about our investigations of the structure of the simple harmonic-repulsive liquid in 3D using the triple correlation function (TCF), i.e., the method that does not rely on the nearest neighbor concept. The liquid is considered at reduced pressure ($P=1.8$) at which it exhibits remarkable stability against crystallization on cooling. It is demonstrated that the TCF allows addressing the development of the orientational correlations in the structures that do not allow drawing definite conclusions from the studies of the bond-orientational order parameters. Our results demonstrate that the orientational correlations, if measured by the heights of the peaks in the TCF, significantly increase on cooling. This rise in the orientational ordering is not captured properly by the Kirkwood's superposition approximation. Detailed considerations of the peaks' shapes in the TCF suggest the existence of a link between the orientational ordering and the slowdown of the system's dynamics. Our findings support the view that the development of the orientational correlations in liquids may play a significant role in the liquids' dynamics and that the considerations of the pair distribution function may not be sufficient to understand intuitively all the structural changes that happen with liquids on supercooling.

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