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Two-order-parameter model of the liquid-glass transition. I. Relation between glass transition and crystallization

机译:液体玻璃化转变的二阶参数模型。一,玻璃化转变与结晶之间的关系

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Recently we proposed a two-order-parameter model of liquid to understand the liquid-glass transition, liquid-liquid transition, and anomalies of water-type liquids in a unified manner. Here we discuss the relation between our model and previous models of the liquid-glass transition, focusing on the difference in the basic standpoint among the models. We argue that (i) actual liquids universally have a tendency of spontaneous formation of locally favored structures and (ii) liquid-glass transition is controlled by the competition between long-range density ordering toward crystallization and short-range bond ordering toward the formation of locally favored structures due to the incompatibility in their symmetry. Thus, we regard vitrification as phenomena that are intrinsically related to crystallization. Previous models, on the other hand, regard vitrification as a result of (a) an homogeneous increase in the density and the resulting cooperativity in molecular motion or (b) the frustration intrinsic to a liquid state itself. Accordingly, they presuppose the kinetic avoidance of crystallization and thus do not put focus on 'crystallization'. This leads to the essential difference in the physical picture between our model and previous models. By comparing models, we aim at gaining further insight into what is the physical origin of the liquid-glass transition and its possible connection with crystallization. (c) 2005 Elsevier B.V. All rights reserved.
机译:最近,我们提出了一种液体的二阶参数模型,以便以统一的方式理解液体玻璃化转变,液体-液体转变和水型液体的异常情况。在这里,我们讨论模型与以前的玻璃液化转变模型之间的关系,着眼于模型之间基本立场上的差异。我们认为(i)实际液体普遍具有自发形成局部偏爱的结构的趋势,并且(ii)液-玻璃化转变受结晶的长程密度有序与结晶的短程键有序之间的竞争控制。由于其对称性不兼容,局部受青睐的结构。因此,我们将玻璃化视为本质上与结晶有关的现象。另一方面,以前的模型认为玻璃化是由于(a)密度均匀提高和分子运动产生的协同作用,或者(b)液态本身固有的挫败感。因此,他们以动力学避免结晶为前提,因此没有把重点放在“结晶”上。这导致我们的模型与以前的模型在物理图像上存在本质的区别。通过比较模型,我们旨在进一步了解液体-玻璃化转变的物理成因及其与结晶的可能联系。 (c)2005 Elsevier B.V.保留所有权利。

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