Abstract

The emergence of glassy dynamics and the glass transition in dense disordered systems is still not fully understood theoretically. Mode-coupling theory (MCT) has shown to be effective in describing some of the non-trivial features of glass formation, but it cannot explain the full glassy phenomenology due to the strong approximations on which it is based. Generalized mode-coupling theory (GMCT) is a hierarchical extension of the theory, which is able to outclass MCT by carefully describing the dynamics of higher-order correlations in its generalized framework. Unfortunately, the theory has so far only been developed for single-component systems and as a result works poorly for highly polydisperse materials. In this paper, we solve this problem by developing GMCT for multi-component systems. We use it to predict the glassy dynamics of the binary Kob–Andersen Lennard-Jones mixture, as well as its purely repulsive Weeks–Chandler–Andersen analogue. Our results show that each additional level of the GMCT hierarchy gradually improves the predictive power of GMCT beyond its previous limit. This implies that our theory is able to harvest more information from the static correlations, thus being able to better understand the role of attraction in supercooled liquids from a first-principles perspective.

Graphic abstract

中文翻译：

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多组分广义模式耦合理论：从玻璃态混合物的结构预测动力学

摘要

玻璃动力学的出现和致密无序系统中的玻璃化转变在理论上仍未完全理解。模式耦合理论 (MCT) 已证明在描述玻璃形成的一些重要特征方面是有效的，但由于它所基于的强近似，它无法解释完整的玻璃现象学。广义模式耦合理论 (GMCT) 是该理论的层次扩展，它能够通过在其广义框架中仔细描述高阶相关性的动力学来超越 MCT。不幸的是，到目前为止，该理论仅针对单组分系统开发，因此对于高度多分散的材料效果不佳。在本文中，我们通过为多组件系统开发 GMCT 来解决这个问题。我们用它来预测二元 Kob-Andersen Lennard-Jones 混合物的玻璃态动力学，以及它纯粹令人厌恶的 Weeks-Chandler-Andersen 类似物。我们的结果表明，GMCT 层次结构的每个附加级别都会逐渐提高 GMCT 的预测能力，使其超出其先前的限制。这意味着我们的理论能够从静态相关性中获取更多信息，从而能够从第一性原理的角度更好地理解吸引力在过冷液体中的作用。

图形摘要