Atomistic characterization of the SiO2 high-density liquid/low-density liquid interface
Atomistic characterization of the SiO2 high-density liquid/low-density liquid interface
复制标题
SiO2 高密度液体/低密度液体界面的原子表征
DOI：
10.1063/5.0107674
复制
发表时间：
2022
影响因子：
4.4
通讯作者：
Y. Yang
中科院分区：
文献类型：
--
作者：
X. Zhang;B. B. Laird;H. T. Liang;W. L. Lu;Z. Y. Yu;X. M. Ma;Y. Cheng;Y. Yang
利用分子动力学模拟研究了高密度液相（HDL）和低密度液相（LDL）之间的平衡二氧化硅液-液界面。的结构，热力学和动力学的界面区域内的详细特征，并与以前的研究相比，在散装二氧化硅的液-液相变（LLPT），以及传统的晶体-熔体界面。我们发现，二氧化硅高密度脂蛋白-低密度脂蛋白界面表现出一个空间的脆弱到强大的过渡整个接口。动力学性质的计算揭示了三种类型的动态异质性杂化内的二氧化硅HDL-LDL接口。我们还观察到，作为接口是从HDL到LDL遍历，Si/O的配位数比跳到一个意想不到的大值，定义了一个薄的区域的接口，HDL和LDL表现出显着的混合。此外，在传统的合金热力学和相平衡的框架下解释了LLPT相共存。
The equilibrium silica liquid-liquid interface between the high-density liquid (HDL) phase and the low-density liquid (LDL) phase is examined using molecular-dynamics simulation. The structure, thermodynamics, and dynamics within the interfacial region are characterized in detail and compared with previous studies on the liquid-liquid phase transition (LLPT) in bulk silica, as well as traditional crystal-melt interfaces. We find that the silica HDL-LDL interface exhibits a spatial fragile-to-strong transition across the interface. Calculations of dynamics properties reveal three types of dynamical heterogeneity hybridizing within the silica HDL-LDL interface. We also observe that as the interface is traversed from HDL to LDL, the Si/O coordination number ratio jumps to an unexpectedly large value, defining a thin region of the interface where HDL and LDL exhibit significant mixing. In addition, the LLPT phase coexistence is interpreted in the framework of the traditional thermodynamics of alloys and phase equilibria.