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颗粒状物理凝胶的结构、力学和振动特性

Structural, mechanical, and vibrational properties of particulate physical gels.

作者信息

Mizuno Hideyuki, Hachiya Makoto, Ikeda Atsushi

机构信息

Graduate School of Arts and Sciences, The University of Tokyo, Tokyo 153-8902, Japan.

出版信息

J Chem Phys. 2021 Dec 21;155(23):234502. doi: 10.1063/5.0072863.

Abstract

Our lives are surrounded by a rich assortment of disordered materials. In particular, glasses are well known as dense, amorphous materials, whereas gels exist in low-density, disordered states. Recent progress has provided a significant step forward in understanding the material properties of glasses, such as mechanical, vibrational, and transport properties. In contrast, our understanding of particulate physical gels is still highly limited. Here, using molecular dynamics simulations, we study a simple model of particulate physical gels, the Lennard-Jones (LJ) gels, and provide a comprehensive understanding of their structural, mechanical, and vibrational properties, all of which are markedly different from those of LJ glasses. First, the LJ gels show sparse, heterogeneous structures, and the length scale ξ of the structures grows as the density is lowered. Second, the LJ gels are extremely soft, with both shear G and bulk K moduli being orders of magnitude smaller than those of LJ glasses. Third, many low-frequency vibrational modes are excited, which form a characteristic plateau with the onset frequency ω in the vibrational density of states. Structural, mechanical, and vibrational properties, characterized by ξ, G, K, and ω, respectively, show power-law scaling behaviors with the density, which establishes a close relationship between them. Throughout this work, we also reveal that LJ gels are multiscale, solid-state materials: (i) homogeneous elastic bodies at long lengths, (ii) heterogeneous elastic bodies with fractal structures at intermediate lengths, and (iii) amorphous structural bodies at short lengths.

摘要

我们的生活被各种各样的无序材料所包围。特别是,玻璃是众所周知的致密无定形材料,而凝胶则处于低密度无序状态。最近的进展在理解玻璃的材料特性方面向前迈出了重要一步,比如机械、振动和传输特性。相比之下,我们对颗粒物理凝胶的理解仍然非常有限。在这里,我们使用分子动力学模拟研究颗粒物理凝胶的一个简单模型—— Lennard-Jones(LJ)凝胶,并全面了解它们的结构、机械和振动特性,所有这些特性都与LJ玻璃的特性明显不同。首先,LJ凝胶呈现出稀疏、不均匀的结构,并且结构的长度尺度ξ随着密度的降低而增大。其次,LJ凝胶极其柔软,剪切模量G和体积模量K都比LJ玻璃小几个数量级。第三,许多低频振动模式被激发,这些模式在振动态密度中形成一个以起始频率ω为特征的平台。分别以ξ、G、K和ω为特征的结构、机械和振动特性呈现出与密度的幂律标度行为,这在它们之间建立了紧密的关系。在整个研究过程中,我们还揭示了LJ凝胶是多尺度固态材料:(i)在长尺度上是均匀弹性体,(ii)在中间尺度上是具有分形结构的非均匀弹性体,(iii)在短尺度上是无定形结构体。

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