论文标题

多体相关性在脆弱和强玻璃形式中都是不可忽略的

Many-body correlations are non-negligible in both fragile and strong glassformers

论文作者

Luo, Chengjie, Robinson, Joshua F., Pihlajamaa, Ilian, Debets, Vincent E., Royall, C. Patrick, Janssen, Liesbeth M. C.

论文摘要

人们普遍认为,慢速玻璃动力学的出现是在材料的微观结构中编码的。第一原理理论[模式耦合理论(MCT)]能够预测仅静态两点相关性作为输入的动力学的急剧减慢,但它无法捕获所有观察到的动力学行为。在这里,我们通过系统地扩展MCT以包含高阶静态和动态相关性来超越两点空间相关函数。我们证明,仅添加静态三重直接相关性已经在定性上改变了预测的二进制硬球和二氧化硅的玻璃传输图。此外,我们发现静态三重相关性之间的竞争是稳定玻璃状态的静态三重相关性与动态的高阶相关性,使两种材料对其稳定。我们得出的结论是,通常在脆弱和强玻璃形式中,常规被忽视的静态三胞胎直接相关以及高阶动态相关性实际上是不可忽略的。

It is widely believed that the emergence of slow glassy dynamics is encoded in a material's microstructure. First-principles theory [mode-coupling theory (MCT)] is able to predict the dramatic slowdown of the dynamics from only static two-point correlations as input, yet it cannot capture all of the observed dynamical behavior. Here we go beyond two-point spatial correlation functions by extending MCT systematically to include higher-order static and dynamic correlations. We demonstrate that only adding the static triplet direct correlations already qualitatively changes the predicted glass-transition diagram of binary hard spheres and silica. Moreover, we find a non-trivial competition between static triplet correlations that work to stabilize the glass state, and dynamic higher-order correlations which destabilize it for both materials. We conclude that the conventionally neglected static triplet direct correlations as well as higher-order dynamic correlations are in fact non-negligible in both fragile and strong glassformers.

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