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Dynamically correlated regions and configurational entropy in supercooled liquids

机译:过冷液体中的动态相关区域和构型熵

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摘要

When a liquid is cooled below its melting temperature, if crystallization is avoided, it forms a glass. Thisphenomenon, called glass transition, is characterized by a marked increase of viscosity, about 14 orders ofmagnitude, in a narrow temperature interval. The microscopic mechanism behind the glass transition is stillpoorly understood. However, recently, great advances have been made in the identification of cooperatiVerearranging regions, or dynamical heterogeneities, i.e., domains of the liquid whose relaxation is highlycorrelated. The growth of the size of these domains is now believed to be the driving mechanism for theincrease of the viscosity. Recently a tool to quantify the size of these domains has been proposed. We applythis tool to a wide class of materials to investigate the correlation between the size of the heterogeneities andtheir configurational entropy, i.e., the number of states accessible to a correlated domain. We find that therelaxation time of a given system, apart from a material dependent prefactor, is a uniVersal function of theconfigurational entropy of a correlated domain. As a consequence, we find that, at the glass transitiontemperature, the size of the domains and the configurational entropy per unit volume are anticorrelated, asoriginally predicted by the Adam-Gibbs theory. Finally, we use our data to extract some exponents definedin the framework of the random first-order theory, a recent quantitative theory of the glass transition.
机译:当液体冷却到低于其熔融温度时,如果避免结晶,则形成玻璃。这种现象称为玻璃化转变,其特征是在狭窄的温度区间内粘度显着增加,约为14个数量级。人们对玻璃化转变背后的微观机理还知之甚少。然而,近来,在确定协同工作的重排区域或动态异质性,即弛豫高度相关的液体域方面已取得了很大的进展。这些域的大小的增长现在被认为是粘度增加的驱动机制。最近,提出了一种量化这些域大小的工具。我们将此工具应用于各种材料,以研究异质性大小与其构型熵之间的相关性,即相关域可访问的状态数。我们发现,给定系统的弛豫时间除依赖物质的因素外,还是相关域的配置熵的通用函数。结果,我们发现,在玻璃化转变温度下,畴的大小与单位体积的构型熵是反相关的,这是由Adam-Gibbs理论最初预测的。最后,我们使用我们的数据提取在随机一阶理论(最近的玻璃化转变定量理论)的框架中定义的一些指数。

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