Revealing the relationship between liquid fragility and medium-range order in silicate glasses.
Revealing the relationship between liquid fragility and medium-range order in silicate glasses.
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DOI：
10.1038/s41467-022-35711-6
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发表时间：
2023-01-03
影响因子：
16.6
通讯作者：
Allan, Douglas C.
中科院分区：
文献类型：
--
作者：
Shi, Ying;Deng, Binghui;Gulbiten, Ozgur;Bauchy, Mathieu;Zhou, Qi;Neuefeind, Joerg;Elliott, Stephen R.;Smith, Nicholas J.;Allan, Douglas C.
尽管经过几十年的研究，玻璃化转变的本质仍然难以捉摸。特别是，在玻璃化转变的动态逮捕的熔体的尖锐性是由其脆弱性。在这里，我们发现，脆弱性是由中程秩序结构。基于一系列铝硅酸盐玻璃的中子衍射数据，我们提出了一个可测量的结构参数，具有很强的反相关性与脆弱性，即平均中程距离（MRD）。我们使用原位高温中子散射数据来讨论这种相关性的物理起源。我们认为，表现出低MRD值的玻璃呈现出过量的小网络环。这种环不稳定，随着温度的变化更容易变形，这往往会增加脆弱性。这些结果表明，硅酸盐玻璃在玻璃化转变时所经历的动态停滞的尖锐性令人惊讶地编码到其网络中的环的稳定性中。脆性描述了熔体在其玻璃化转变时动力学停滞的尖锐性，但其结构起源仍然难以捉摸。Shi等人的研究表明，脆弱性与中程有序结构呈负相关，其特征是一个可测量的参数，称为平均中程距离。
Despite decades of studies, the nature of the glass transition remains elusive. In particular, the sharpness of the dynamical arrest of a melt at the glass transition is captured by its fragility. Here, we reveal that fragility is governed by the medium-range order structure. Based on neutron-diffraction data for a series of aluminosilicate glasses, we propose a measurable structural parameter that features a strong inverse correlation with fragility, namely, the average medium-range distance (MRD). We use in-situ high-temperature neutron-scattering data to discuss the physical origin of this correlation. We argue that glasses exhibiting low MRD values present an excess of small network rings. Such rings are unstable and deform more readily with changes in temperature, which tends to increase fragility. These results reveal that the sharpness of the dynamical arrest experienced by a silicate glass at the glass transition is surprisingly encoded into the stability of rings in its network. Fragility describes the sharpness of dynamical arrest of a melt at its glass transition, yet its structural origin remains elusive. Shi et al. show that fragility inversely correlates with the medium-range order structure characterized by a measurable parameter named the average medium-range distance.
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DOI：
10.1073/pnas.1503741112
发表时间：
2015-11-10
影响因子：
11.1
作者：
Krausser, Johannes;Samwer, Konrad H.;Zaccone, Alessio
通讯作者：
Zaccone, Alessio
DOI：
10.1073/pnas.0911705106
发表时间：
2009-11-24
影响因子：
11.1
作者：
Mauro, John C.;Yue, Yuanzheng;Allan, Douglas C.
通讯作者：
Allan, Douglas C.
影响因子：
4.4
作者：
Hermansen, Christian;Mauro, John C.;Yue, Yuanzheng
通讯作者：
Yue, Yuanzheng
影响因子：
2.4
作者：
Novikov, V. N.
通讯作者：
Novikov, V. N.
影响因子：
3.5
作者：
Moesgaard, Mette;Yue, Yuanzheng
通讯作者：
Yue, Yuanzheng