Department of Chemistry, Physical and Theoretical Chemistry Laboratory, University of Oxford, South Parks Road, Oxford OX1 3QZ, United Kingdom.
Phys Rev Lett. 2009 Oct 9;103(15):157801. doi: 10.1103/PhysRevLett.103.157801. Epub 2009 Oct 7.
Network-forming liquids comprising tetrahedral motifs are investigated by large-scale molecular dynamics computer simulations within the framework of an ionic interaction model. The network topology is controlled by varying the anion polarizability, which governs the intertetrahedral bond angle, for different system densities. A coupling is found between the growth in magnitude and range of extended range oscillations and the appearance of ordering on an intermediate length scale. The interrelation between the system fragility and the structural arrangements on these two different length scales shows the trends that are observed for glass-forming systems. In particular, the fragility increases with number of edge-sharing motifs.
采用离子相互作用模型,通过大规模分子动力学计算机模拟研究了由四面体结构基元组成的网络形成液体。通过改变阴离子极化率来控制网络拓扑结构,从而控制不同体系密度下的四面体键角。研究发现,在中等长度尺度上,扩展范围振荡的幅度和范围的增加与有序性的出现之间存在耦合关系。系统脆性与这两个不同长度尺度上结构排列之间的相互关系显示了玻璃形成系统中观察到的趋势。特别是,脆性随棱边共享基元数量的增加而增加。