Jakse Noël, Alvares Cecilia M S, Pisch Alexander
Université Grenoble Alpes, CNRS, Grenoble INP, SIMaP, F-38000 Grenoble, France.
J Phys Condens Matter. 2021 May 31;33(28). doi: 10.1088/1361-648X/abfc0f.
Calcium aluminotitanate (CaO-AlO-TiO) ternary oxides are of fundamental interest in Materials as well as Earth and environmental science, and a key system for several industrial applications. As their properties at the atomic scale are scarcely known, interionic interactions for the melts are built from a bottom up strategy consisting in fitting first only AlO, CaO and TiOsingle oxide compounds separately with a unified description of the oxygen charge and O-O interaction term. For this purpose, a mean-square difference minimization of the partial pair-correlation functions with respect to thereference was performed. The potentials for the ternary oxide are finally built straightforwardly by adding purely Coulomb terms for dissimilar cation-cation interactions without further fit. This general and unified approach is transferable and successfully describes the structural and diffusion properties of the three single oxides as well as the ternary melts simultaneously. A possible underlying structural mechanism at the origin of the diffusion evolution with TiOcontent is proposed based on the formation of Ti induced triply bonded oxygen.
铝酸钛钙（CaO-AlO-TiO）三元氧化物在材料科学以及地球与环境科学领域具有重要的基础研究价值，并且是多种工业应用的关键体系。由于其在原子尺度上的性质鲜为人知，因此通过自下而上的策略构建熔体中的离子间相互作用，该策略首先仅分别对AlO、CaO和TiO单一氧化物化合物进行拟合，并统一描述氧电荷和O-O相互作用项。为此，针对参考体系对部分对关联函数进行了均方差最小化处理。三元氧化物的势最终通过添加不同阳离子-阳离子相互作用的纯库仑项直接构建而成，无需进一步拟合。这种通用且统一的方法具有可转移性，并成功地同时描述了三种单一氧化物以及三元熔体的结构和扩散性质。基于Ti诱导的三键氧的形成，提出了TiO含量导致扩散演变的潜在结构机制。
