当前位置:
X-MOL 学术
›
J. Phys. Chem. Lett.
›
论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Short-Range Disorder in TeO2 Melt and Glass.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2019-12-30 , DOI: 10.1021/acs.jpclett.9b03231 O L G Alderman 1 , C J Benmore 2 , S Feller 3 , E I Kamitsos 4 , E D Simandiras 4 , D G Liakos 5 , M Jesuit 3 , M Boyd 3 , M Packard 3 , R Weber 1, 2
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2019-12-30 , DOI: 10.1021/acs.jpclett.9b03231 O L G Alderman 1 , C J Benmore 2 , S Feller 3 , E I Kamitsos 4 , E D Simandiras 4 , D G Liakos 5 , M Jesuit 3 , M Boyd 3 , M Packard 3 , R Weber 1, 2
Affiliation
![]() |
High-resolution X-ray pair distribution functions for molten and glassy TeO2 reveal coordination numbers nTeO ≈ 4. However, distinct from the known α-, β-, and γ-TeO2 polymorphs, there is considerable short-range disorder such that no clear cutoff distance between bonded and nonbonded interactions exists. We suggest that this is similar to disorder in δ-TeO2 and arises from a broad distribution of asymmetric Te-O-Te bridges, something that we observe becomes increasingly asymmetric with increasing liquid temperature. Such behavior is qualitatively consistent with existing interpretations of Raman scattering spectra, and equivalent to temperature-induced coordination number reduction, for sufficiently large cutoff radii. Therefore, TeO2 contains a distribution of local environments that are, furthermore, temperature dependent, making it distinct from the canonical single-oxide glass formers. Our results are in good agreement with high-level ab initio cluster calculations.
中文翻译:
TeO2熔融和玻璃中的短程失调。
熔融和玻璃态TeO2的高分辨率X射线对分布函数揭示了配位数nTeO≈4。但是,与已知的α-,β-和γ-TeO2多晶型物不同,存在相当大的短程无序现象,因此不清楚存在键合和非键合相互作用之间的截止距离。我们建议,这类似于δ-TeO2的无序,并且是由于不对称的Te-O-Te桥的广泛分布引起的,随着液体温度的升高,我们观察到的事情变得越来越不对称。对于足够大的截止半径,这种行为与拉曼散射光谱的现有解释在质量上是一致的,并且等同于温度引起的配位数的减少。因此,TeO2包含与温度有关的局部环境分布,使其与规范的单氧化物玻璃形成剂不同。我们的结果与高级从头算起簇计算非常吻合。
更新日期:2019-12-31
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
TeO2熔融和玻璃中的短程失调。
熔融和玻璃态TeO2的高分辨率X射线对分布函数揭示了配位数nTeO≈4。但是,与已知的α-,β-和γ-TeO2多晶型物不同,存在相当大的短程无序现象,因此不清楚存在键合和非键合相互作用之间的截止距离。我们建议,这类似于δ-TeO2的无序,并且是由于不对称的Te-O-Te桥的广泛分布引起的,随着液体温度的升高,我们观察到的事情变得越来越不对称。对于足够大的截止半径,这种行为与拉曼散射光谱的现有解释在质量上是一致的,并且等同于温度引起的配位数的减少。因此,TeO2包含与温度有关的局部环境分布,使其与规范的单氧化物玻璃形成剂不同。我们的结果与高级从头算起簇计算非常吻合。