Revealing the medium-range structure of glassy silica using force-enhanced atomic refinement
Revealing the medium-range structure of glassy silica using force-enhanced atomic refinement
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DOI：
10.1016/j.jnoncrysol.2021.121138
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发表时间：
2021-12
影响因子：
3.5
通讯作者：
Qi Zhou;Ying Shi;Binghui Deng;T. Du;Lijie Guo;Morten M. Smedskjær;M. Bauchy
中科院分区：
文献类型：
--
作者：
Qi Zhou;Ying Shi;Binghui Deng;T. Du;Lijie Guo;Morten M. Smedskjær;M. Bauchy
硅酸盐玻璃的中程有序结构仍然知之甚少，因为它不能从常规实验中直接看到。反过来，虽然原子模拟提供了对玻璃结构的直接访问，但它们面临着几个限制，例如，极高的冷却速率。在这里，我们采用力增强原子细化（FEAR）的方法来克服这些限制，并揭示玻璃态二氧化硅的原子结构，无论是在短期和中期的长度尺度。我们发现，FEAR产生的玻璃结构，同时表现出更高的热力学稳定性和增强的协议与实验结构数据相比，分子动力学和反向蒙特卡罗模拟。总的来说，我们表明，增加的稳定性，使恐惧主要来自这样一个事实，即所产生的原子配置表现出更有序的中程结构和较低的分数不稳定的小硅酸盐环。
The medium-range order structure of silicate glasses remains poorly known as it is not directly visible from conventional experiments. In turn, although atomistic simulations offer a direct access to the structure of glasses, they face several limitations, e.g., extremely high cooling rates. Here, we adopt the force-enhanced atomic refinement (FEAR) method to overcome these limitations and reveal the atomic structure of glassy silica, both at the short- and medium-range length scales. We find that FEAR yields a glass structure that simultaneously exhibits higher thermodynamic stability and enhanced agreement with experimental structure data as compared with molecular dynamics and reverse Monte Carlo simulations. Overall, we show that the increased stability enabled by FEAR primarily arises from the fact that the generated atomic configuration exhibits a more ordered medium-range structure and a lower fraction of unstable small silicate rings.