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结构玻璃刚性的复制理论。

Replica theory of the rigidity of structural glasses.

机构信息

Department of Earth and Space Science, Faculty of Science, Osaka University, Toyonaka 560-0043, Japan.

出版信息

J Chem Phys. 2012 Jun 7;136(21):214108. doi: 10.1063/1.4722343.

Abstract

We present a first principle scheme to compute the rigidity, i.e., the shear-modulus of structural glasses at finite temperatures using the cloned liquid theory, which combines the replica theory and the liquid theory. With the aid of the replica method which enables disentanglement of thermal fluctuations in liquids into intra-state and inter-state fluctuations, we extract the rigidity of metastable amorphous solid states in the supercooled liquid and glass phases. The result can be understood intuitively without replicas. As a test case, we apply the scheme to the supercooled and glassy state of a binary mixture of soft-spheres. The result compares well with the shear-modulus obtained by a previous molecular dynamic simulation. The rigidity of metastable states is significantly reduced with respect to the instantaneous rigidity, namely, the Born term, due to non-affine responses caused by displacements of particles inside cages at all temperatures down to T = 0. It becomes nearly independent of temperature below the Kauzmann temperature T(K). At higher temperatures in the supercooled liquid state, the non-affine correction to the rigidity becomes stronger suggesting melting of the metastable solid state. Inter-state part of the static response implies jerky, intermittent stress-strain curves with static analogue of yielding at mesoscopic scales.

摘要

我们提出了一种基于克隆液体理论的第一性原理方案,用于计算结构玻璃在有限温度下的刚性,即剪切模量。该理论结合了复制理论和液体理论。借助复制方法,可以将液体中的热波动分解为内态和外态波动,从而提取出过冷液体和玻璃相中亚稳非晶态的刚性。该结果无需复制即可直观理解。作为一个测试案例,我们将该方案应用于软球二元混合物的过冷和玻璃态。结果与先前分子动力学模拟得到的剪切模量非常吻合。由于在所有温度下(直至 T=0)粒子在笼内的位移引起的非仿射响应,亚稳态的刚性相对于瞬时刚性(即 Born 项)显著降低。在低于 Kauzmann 温度 T(K)的温度下,它几乎与温度无关。在过冷液体状态下的较高温度下,对刚性的非仿射修正变得更强,表明亚稳固相的熔化。静态响应的外态部分意味着在介观尺度上具有突跳式、间歇性的应力-应变曲线以及静态屈服类似物。

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