Institute of Energy and Climate Research, Nuclear Waste Management and Reactor Safety, Forschungszentrum Jülich, Wilhelm-Johnen-Strasse, 52428, Jülich, Germany; JARA High-Performance Computing, Schinkelstrasse 2, 52062, Aachen, Germany.
J Comput Chem. 2014 Jul 5;35(18):1339-46. doi: 10.1002/jcc.23618. Epub 2014 Apr 24.
We performed a density functional theory (DFT) study of the monazite-type ceramics using DFT+U method, where the Hubbard U parameters are derived ab initio, with the main goal in testing the predictive power of this computational method for modeling of f-electron materials that are of interest in nuclear waste management. We show that DFT+U approach with PBEsol as the exchange-correlation functional significantly improves description of structures and thermodynamic parameters of lanthanide-bearing oxides and monazites over commonly used standard DFT (PBE) approach. We found that it is essential to use the Hubbard U parameter derived for a given element and a given structure to reproduce the structural parameters of the measured materials. We obtained exceptionally good description of the structural parameters with U parameter derived using the linear response approach of Cococcioni and de Gironcoli (Phys. Rev. B 2005, 71, 035105). This shows that affordable methods, such as DFT+U with a clever choice of exchange-correlation functional and the Hubbard U parameter can lead to a good description of f-electron materials.
我们使用密度泛函理论（DFT）+U 方法对独居石型陶瓷进行了研究，其中 Hubbard U 参数是从头算得出的，主要目的是测试这种计算方法对核废料管理中感兴趣的 f 电子材料建模的预测能力。我们表明，使用 PBEsol 作为交换相关泛函的 DFT+U 方法显著改善了含镧氧化物和独居石的结构和热力学参数的描述，优于常用的标准 DFT（PBE）方法。我们发现，对于给定的元素和结构，使用为给定元素和结构推导的 Hubbard U 参数来重现测量材料的结构参数是至关重要的。我们使用 Cococcioni 和 de Gironcoli 的线性响应方法（Phys. Rev. B 2005, 71, 035105）得出的 U 参数，对结构参数进行了异常良好的描述。这表明，诸如 DFT+U 与巧妙选择交换相关泛函和 Hubbard U 参数等经济适用的方法可以导致对 f 电子材料的良好描述。
