Viscosity of glass-forming liquids
Viscosity of glass-forming liquids
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DOI：
10.1073/pnas.0911705106
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发表时间：
2009-11-24
影响因子：
11.1
通讯作者：
Allan, Douglas C.
中科院分区：
文献类型：
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作者：
Mauro, John C.;Yue, Yuanzheng;Allan, Douglas C.
超高压液体的低温动力学是理解玻璃化转变和弛豫现象的本质的关键，包括理想热力学玻璃化转变的潜在存在。不幸的是，现有的粘度模型，如VFT （Vogel-Fulcher-Tammann）和Avramov-Milchev （AM）方程，在推断低温时表现出系统误差。我们提出了一个模型，使用与VFT和AM相同数量的参数，对无机和有机液体的粘度-温度关系进行了改进的描述。该模型基于构型熵的温度依赖性，具有明确的物理基础，能够准确预测有限温度下的低温等温线，且无奇点。我们的结果对Kauzmann熵突变和相关理想玻璃化转变的存在提出了质疑。
The low-temperature dynamics of ultraviscous liquids hold the key to understanding the nature of glass transition and relaxation phenomena, including the potential existence of an ideal thermodynamic glass transition. Unfortunately, existing viscosity models, such as the Vogel-Fulcher-Tammann (VFT) and Avramov-Milchev (AM) equations, exhibit systematic error when extrapolating to low temperatures. We present a model offering an improved description of the viscosity-temperature relationship for both inorganic and organic liquids using the same number of parameters as VFT and AM. The model has a clear physical foundation based on the temperature dependence of configurational entropy, and it offers an accurate prediction of low-temperature isokoms without any singularity at finite temperature. Our results cast doubt on the existence of a Kauzmann entropy catastrophe and associated ideal glass transition.