论文标题

johari-goldstein $β$玻璃动力学的放松源自两尺度的能量景观

Johari-Goldstein $β$ relaxation in glassy dynamics originates from two-scale energy landscape

论文作者

Shiraishi, Kumpei, Mizuno, Hideyuki, Ikeda, Atsushi

论文摘要

超冷的液体会经历复杂的结构放松过程,这在凝结物理物理学的实验和理论方面都是一个长期存在的问题。特别是,对于许多类型的分子液体,人们普遍观察到的过去实验,这些液体在低温下分为两个不同的过程。可能的解释之一是,这种分离起源于势能景观的两个规模分层地形。但是,它从未得到过验证。分子动力学模拟是解决此问题的一种有前途的方法,但我们必须克服艰辛的困难。首先,我们必须处理与简单的球形模型相比,该模型在计算上要求,该模型经过深入研究,但仅显示一个较慢的过程:$α$放松。其次,我们必须达到一个足够低温的状态,这两个过程变得很好分开。在这里,我们处理一个不对称的二聚体系统,该系统表现出更快的过程:Johari-Goldstein $β$放松。然后,我们采用平行回火方法来访问低温方案。这些费力的努力使我们能够详细研究势能格局,并揭示了诱导$β$放松的地形层次结构的第一个直接证据。我们还成功地表征了每个放松过程中颗粒的微观运动。最后,我们研究了两个放松过程的低频模式的预测能力。我们的结果首次建立了对超冷液体中实验观察到的放松动态的基本和全面的理解。

Supercooled liquids undergo complicated structural relaxation processes, which have been a long-standing problem in both experimental and theoretical aspects of condensed matter physics. In particular, past experiments universally observed for many types of molecular liquids that relaxation dynamics separated into two distinct processes at low temperatures. One of the possible interpretations is that this separation originates from the two-scale hierarchical topography of the potential energy landscape; however, it has never been verified. Molecular dynamics simulations are a promising approach to tackle this issue, but we must overcome laborious difficulties. First, we must handle a model of molecular liquids that is computationally demanding compared to simple spherical models, which have been intensively studied but show only a slower process: $α$ relaxation. Second, we must reach a sufficiently low-temperature regime where the two processes become well separated. Here, we handle an asymmetric dimer system that exhibits a faster process: Johari-Goldstein $β$ relaxation. Then, we employ the parallel tempering method to access the low-temperature regime. These laborious efforts enable us to investigate the potential energy landscape in detail and unveil the first direct evidence of the topographic hierarchy that induces the $β$ relaxation. We also successfully characterize the microscopic motions of particles during each relaxation process. Finally, we study the predictive power of low-frequency modes for two relaxation processes. Our results establish for the first time a fundamental and comprehensive understanding of experimentally observed relaxation dynamics in supercooled liquids.

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