论文标题

广义模式耦合理论的玻璃动力学:用于层次耦合的整体差异方程的解决方案的存在和独特性

Glassy dynamics from generalized mode-coupling theory: existence and uniqueness of solutions for hierarchically coupled integro-differential equations

论文作者

Biezemans, Rutger A., Ciarella, Simone, Çaylak, Onur, Baumeier, Björn, Janssen, Liesbeth M. C.

论文摘要

广义模式耦合理论(GMCT)是一种基于第一原理的,系统地更正的框架,可预测玻璃形成材料的复杂松弛动力学。正式理论相当于无限多个耦合的整体差异方程的层次结构,可以使用合适的有限级闭合关系来近似。尽管先前的研究表明有限级GMCT导致了明确的溶液,并且随着闭合水平的增加,层次结构会收敛,但已知在这个方向上尚无严格和一般的结果。在这里,我们明确地确定了以任意顺序关闭的通用示意性GMCT层次结构的解决方案的存在和独特性。我们考虑了两种通常调用的闭合近似值,即均值场和指数闭合。我们还明确区分了过度阻尼和阻尼不足的玻璃动力学,分别对应于一阶和二阶不差异方程的层次结构。我们发现,截断的GMCT层次结构在指数闭合符合先前开发的数学理论的构成下关闭,因此可以很容易地推断出独特解决方案的存在。然而,自一致的平均景点封闭,其中众所周知的标准-MCT闭合近似是一种特殊情况,需要对数学严谨的其他论点。我们证明,解决方案上的先验界限的存在足以证明这种自洽的层次结构存在独特的解决方案。为了完成我们的分析,我们提出了简单的论点,以表明必须存在这些先验界限,这是由GMCT解决方案作为密度相关函数的物理解释所激发的。总体而言,我们的工作有助于GMCT的理论理由,用于研究玻璃过渡,将GMCT置于更牢固的数学基础上。

Generalized mode-coupling theory (GMCT) is a first-principles-based and systematically correctable framework to predict the complex relaxation dynamics of glass-forming materials. The formal theory amounts to a hierarchy of infinitely many coupled integro-differential equations, which may be approximated using a suitable finite-order closure relation. Although previous studies have suggested that finite-order GMCT leads to well-defined solutions, and that the hierarchy converges as the closure level increases, no rigorous and general result in this direction is known. Here we unambiguously establish the existence and uniqueness of solutions to generic, schematic GMCT hierarchies that are closed at arbitrary order. We consider two types of commonly invoked closure approximations, namely mean-field and exponential closures. We also distinguish explicitly between overdamped and underdamped glassy dynamics, corresponding to hierarchies of first-order and second-order integro-differential equations, respectively. We find that truncated GMCT hierarchies closed under an exponential closure conform to previously developed mathematical theories, such that the existence of a unique solution can be readily inferred. Self-consistent mean-field closures, however, of which the well-known standard-MCT closure approximation is a special case, warrant additional arguments for mathematical rigour. We demonstrate that the existence of a priori bounds on the solution is sufficient to also prove that unique solutions exist for such self-consistent hierarchies. To complete our analysis, we present simple arguments to show that these a priori bounds must exist, motivated by the physical interpretation of the GMCT solutions as density correlation functions. Overall, our work contributes to the theoretical justification of GMCT for studies of the glass transition, placing GMCT on a firmer mathematical footing.

扫码加入交流群

加入微信交流群

微信交流群二维码

扫码加入学术交流群,获取更多资源