SiO2网络结构的分子模拟及玻璃化研究
Molecular Simulation and Vitrification of SiO2 Network Structure
DOI: 10.12677/MS.2020.1012118, PDF,   
作者: 许浩洋, 刘 俊, 吴荣亮*：东华大学，纤维材料改性国家重点实验室，材料科学与工程学院，上海；杨小震：中国科学院化学研究所，高分子物理与化学国家重点实验室，北京
关键词: 分子模拟；网络结构；玻璃化；协作重排；Molecular Dynamics Simulation； Network Structure； Glass Transition； Cooperational Rearrangement
摘要: 玻璃是一种无序的材料，缺乏晶体的周期性，但在机械性能上类似固体。制作玻璃最常见的方法是快速冷却粘性液体以避免结晶，尽管冷却获得玻璃这一方法已为人们所熟知，但从液体转变成无定型刚性结构这一过程的微观机理还尚未被人们完全理解。经典分子动力学模拟作为一种研究物质微观结构的有效手段，能够提供关于非晶材料静态结构和动态特性的详细信息，为研究玻璃结构提供了科学可行的方法。在本工作中，我们针对以往玻璃分子动力学模拟中无拓扑定义力场对高温和常温下物理性质描述无法兼顾的难题，提出了一种变温拓扑构造方法，在不同的温度下构建不同的SiO2无规网络拓扑结构用于熔体冷却玻璃化过程的分子动力学模拟。分析了熔体冷却玻璃化过程中的结构性质、动力学性质与热力学性质变化，我们发现变温拓扑构造方法能准确描述SiO2玻璃化过程中径向分布函数、体积、扩散系数、松弛时间等结构性质和动力学性质，并且对动力学与热力学关系的描述符合Adam-Gibbs理论，得到的协作重排区域尺寸在熔体冷却玻璃化过程中逐渐减小。
Abstract: Glass is an amorphous material which lacks the periodicity of crystals and behaves as solid in mechanical properties. The most common method to make glass is cooling the viscous liquid quickly to avoid crystallization. Although the method of obtaining glass by cooling is well known, the microscopic mechanism of the transition from liquid to amorphous rigid structure is not fully understood. As an effective means to study the microstructure of materials, classical molecular dynamics simulation can provide detailed information about the static structure and dynamic characteristics of amorphous materials and give the scientific and feasible method for the study of glass structure. In this work, we aim at the problem that the same force field cannot describe the physical properties at high temperature and normal temperature in the previous glass molecular dynamics simulation simultaneously. A method of topological construction of variable temperature was proposed by us, and various topological structures of SiO2 random network were obtained at different temperatures for molecular dynamics simulation of melt cooling vitrification process. The changes of structural properties, kinetic properties and thermodynamic properties in melt cooling vitrification process were analyzed. It is found that the variable temperature topological construction method can accurately describe the variation law of structural properties and dynamic properties such as radial distribution function, volume, diffusion coefficient and relaxation time with temperature in SiO2 vitrification process, and the description of the relationship between dynamics and thermodynamics in vitrification conforms to Adam-Gibbs theory.
文章引用：许浩洋, 刘俊, 吴荣亮, 杨小震. SiO2网络结构的分子模拟及玻璃化研究[J]. 材料科学, 2020, 10(12): 980-992. https://doi.org/10.12677/MS.2020.1012118

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