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Non-equilibrium entropy of glasses formed by continuous cooling

机译:连续冷却形成的玻璃的非平衡熵

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摘要

We propose a generalized definition of entropy accounting for the continuous breakdown of ergodicity at the laboratory glass transition. Our approach is applicable through all regimes of glass forming, from the equilibrium liquid state through the glass transition range and into the glassy state at low temperatures. The continuous loss of ergodicity during the laboratory glass transition is accompanied by a loss of entropy as the system gradually becomes trapped in a subset of the configurational phase space. Using a hierarchical master equation approach, we compute the configurational entropy of selenium, a simple but realistic glass-former, for cooling rates covering 25 orders of magnitude, viz., 10~-12 to 10~12 K/s. In all cases, the entropy of glass is zero in the limit of absolute zero temperature, since here the system is nec_essarily confined to a single microstate.
机译:我们提出了熵的广义定义,以解释实验室玻璃化转变时遍历性的连续分解。我们的方法适用于所有玻璃成形方式,从平衡液态到玻璃态转变范围,再到低温下变成玻璃态。随着系统逐渐陷入结构相空间的一个子集中,实验室玻璃化转变期间遍历性的连续损失伴随着熵的损失。使用分层主方程方法,我们计算出硒的结构熵,这是一种简单而现实的玻璃形成剂,其冷却速率涵盖25个数量级,即10〜-12至10〜12 K / s。在所有情况下,玻璃的熵在绝对零温度的极限内为零,因为在这里,系统必须限制在一个微状态。

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