Can any liquid be cooled down below its melting point to an isentropic (Kauzmann) temperature without vitrifying or crystallizing? This long-standing question concerning the ultimate fate of supercooled liquids is one of the key problems in condensed matter physics and materials science. In this article, we used a plethora of thermodynamic and kinetic data and well established theoretical models to estimate the kinetic spinodal temperature, T_KS (the temperature where the average time for the first critical crystalline nucleus to appear becomes equal to the average relaxation time of a supercooled liquid), and the Kauzmann temperature, T_K, for two substances. We focused our attention on selected compositions of the two most important oxide glass-forming systems: a borate and a silicate—which show measurable homogeneous crystal nucleation in laboratory time scales—as proxies of these families of glass-formers. For both materials, we found that the T_KS are significantly higher than the predicted T_K. Therefore, at ambient pressure, at deep supercoolings before approaching T_K, crystallization wins the race over structural relaxation. Hence, the temperature of entropy catastrophe predicted by Kauzmann cannot be reached for the studied substances; it is averted by incipient crystal nucleation. Our finding that T_KS > T_K for two real glasses corroborate the results of computer simulations for a pressurized silica glass.

中文翻译：

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过冷液体中的竞争—松弛与结晶

是否可以将任何液体冷却至低于其熔点至等熵（Kauzmann）温度，而不会玻璃化或结晶？这个关于过冷液体最终命运的长期存在的问题是凝聚态物理和材料科学中的关键问题之一。在本文中，我们使用了大量的热力学和动力学数据，并建立了完善的理论模型来估算动力学旋节线温度T _KS（第一个关键晶核出现的平均时间等于平均弛豫时间的温度）。过冷的液体）和考兹曼温度T _K，用于两种物质。我们将注意力集中在两个最重要的氧化物玻璃形成系统（硼酸盐和硅酸盐）的选定成分上，它们在这些实验室时间尺度上均显示出可测量的均质晶体成核，以此作为这些玻璃形成者家族的代理。对于这两种材料，我们发现，牛逼_KS是显著高于比预测牛逼_ķ。因此，在环境压力下，在接近T _K之前的深度过冷处，结晶赢得了结构弛豫的竞争。因此，所研究的物质无法达到考兹曼预测的熵突变温度。最初的晶体成核避免了它。我们发现，牛逼_KS > T _K代表两副真实玻璃，证实了加压石英玻璃的计算机模拟结果。