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New scaling paradigm for dynamics in glass-forming systems
Progress in Materials Science ( IF 37.4 ) Pub Date : 2023-01-16 , DOI: 10.1016/j.pmatsci.2023.101074
Aleksandra Drozd-Rzoska , Sylwester J. Rzoska , Szymon Starzonek

The lack of ultimate scaling relations for previtreous changes of the primary relaxation time or viscosity in glass-forming systems constitutes the grand fundamental challenge, also hindering the development of relevant material engineering applications. The report links the problem to the location of the previtreous domain remote from a hypothetical divergence, hidden in the solid glass state. As the solution, the distortions-sensitive and linearized derivative-based analysis is proposed. It is implemented to scaling relations being checkpoints of basic glass transition models: free volume, entropic, critical-like, avoided criticality, kinetically constrained, or Ising model related. For discussed scaling relations, alternative formulations based on fragility, the semi-universal metric for previtreous dynamics, are presented. The alternative approach based on the activation energy index, showing its relative changes, is also presented. Derived relations are validated for the primary relaxation time experimental data in the homologous series of polyols, from glycerol to sorbitol. Only two scaling equations passed the exam: MYEGA, the recent ‘activation and critical’ (AC), and their pressure counterparts. The report shows that the coherent picture linking (i) the Super-Arrhenius for the temperature path, (ii) the Super-Barus behavior for the pressure path, and anomalous changes detected on compessing, namely (iii) inflection, and (iv) viscosity decrease or speeding for relaxation time, is possible.

The report also shows the limited reliability of the so-called Stickel analysis and its pressure counterpart used for detecting the dynamic crossover in the previtreous domain.



中文翻译:

玻璃成型系统动力学的新标度范式

玻璃形成系统中主要弛豫时间或粘度的先前变化缺乏最终标度关系构成了重大的基本挑战,也阻碍了相关材料工程应用的发展。该报告将问题与远离假设分歧的前玻璃域的位置联系起来,隐藏在固态玻璃状态中。作为解决方案,提出了基于失真敏感和线性化导数的分析。它被实施为作为基本玻璃化转变模型检查点的缩放关系:自由体积、熵、临界样、避免临界、动力学约束或伊辛模型相关。对于讨论的比例关系,提出了基于脆弱性的替代公式,即前玻璃体动力学的半通用度量。还介绍了基于显示其相对变化的活化能指数的替代方法。从甘油到山梨糖醇的同源多元醇系列中的主要弛豫时间实验数据验证了派生关系。只有两个比例方程通过了考试:MYEGA、最近的“激活和临界”(AC) 及其对应的压力方程。报告显示,连贯图片将 (i) 温度路径的 Super-Arrhenius,(ii) 压力路径的 Super-Barus 行为,以及压缩时检测到的异常变化,即 (iii) 拐点,和 (iv)粘度降低或弛豫时间加快是可能的。从甘油到山梨糖醇的同源多元醇系列中的主要弛豫时间实验数据验证了派生关系。只有两个比例方程通过了考试:MYEGA、最近的“激活和临界”(AC) 及其对应的压力方程。报告显示,连贯图片将 (i) 温度路径的 Super-Arrhenius,(ii) 压力路径的 Super-Barus 行为,以及压缩时检测到的异常变化,即 (iii) 拐点,和 (iv)粘度降低或弛豫时间加快是可能的。从甘油到山梨糖醇的同源多元醇系列中的主要弛豫时间实验数据验证了派生关系。只有两个比例方程通过了考试:MYEGA、最近的“激活和临界”(AC) 及其对应的压力方程。报告显示,连贯图片将 (i) 温度路径的 Super-Arrhenius,(ii) 压力路径的 Super-Barus 行为,以及压缩时检测到的异常变化,即 (iii) 拐点,和 (iv)粘度降低或弛豫时间加快是可能的。

该报告还显示了所谓的 Stickel 分析及其压力对应物的可靠性有限,该分析用于检测前玻璃域中的动态交叉。

更新日期:2023-01-20
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