玻璃杯的剩余熵藏在哪里？
Where is the residual entropy of a glass hiding?
摘要：
我们重新讨论了Goldstein最近在本期刊[J. Chem. Phys. 128，154510（2008）]中讨论的争论，即剩余熵是真实的还是虚构的。结果表明，玻璃化转变时的剩余熵损失猜想（ELC）导致了熵的不连续性，它违反了经典热力学的许多基本原理，也与一些实验事实相矛盾。假设，在该领域是常见的，玻璃是在内部平衡，我们表明，在玻璃化转变的焓和体积的连续性需要的吉布斯自由能和熵的连续性，这与ELC相矛盾。然后，有人认为，ELC是建立在一个不正确的理解是什么意思的玻璃动力学被困在一个盆地和概率和熵的概念。在我们的方法中，根据再现性原理（见第二节），通过正确地把熵确定为系综熵，一旦纠正了这种误解，就可以立即得出结论，在动力学冻结的玻璃态中，剩余熵不会消失，所有的热力学违反都消失了。我们表明，熵的时间定义在有限的时间没有意义的眼镜，因为它不是唯一的。与最近的一些主张相反，遍历性和因果关系没有损失。
英文摘要：
We revisit the controversy, discussed recently by Goldstein in this journal[J. Chem. Phys. 128,154510 (2008)], whether the residual entropy is real or fictional. It is shown that the residual entropy loss conjecture (ELC) at the glass transition, which results in a discontinuous entropy violates many fundamental principles of classical thermodynamics, and also contradicts some experimental facts. Assuming, as is common in the field, that glasses are in internal equilibrium, we show that the continuity of enthalpy and volume at the glass transition require the continuity of the Gibbs free energy and the entropy, which contradicts ELC. It is then argued that ELC is founded on an incorrect understanding of what it means for a glass to be kinetically trapped in a basin and of the concept of probability and entropy. Once this misunderstanding is corrected in our approach by the proper identification of entropy as the ensemble entropy, which is in accordance with the principle of reproducibility (see Sect. II), it follows immediately that the residual entropy does not disappear in a kinetically frozen glassy state and all the violations of thermodynamics disappear. We show that the temporal definition of entropy over finite times does not make sense for glasses as it is not unique. There is no loss of ergodicity and causality, contrary to some recent claims.
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