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Critical Assessment of the DFT + U Approach for the Prediction of Vanadium Dioxide Properties
Journal of Computational Chemistry ( IF 3.4 ) Pub Date : 2019-11-11 , DOI: 10.1002/jcc.26096
Berenike Stahl 1, 2 , Thomas Bredow 1
Affiliation  

In a previous study (Stahl and Bredow, Chem. Phys. Lett. 2018, 695, 28–33), we have studied structural, energetic, and electronic properties of two vanadium dioxide VO2 polymorphs with modified global and range‐separated hybrid functionals. Since hybrid methods are computationally demanding, we evaluate the computationally more efficient DFT + U method in the present study. We assessed the widely used Dudarev PBE + U approach with a literature value of the effective Hubbard parameter Ueff = 3.4 eV. We compared the PBE + U results for the two VO2 polymorphs with our previous results, a self‐consistent hybrid functional sc‐PBE0, and the meta‐GGA functional SCAN. It was found that the PBE + U method yields a strongly distorted monoclinic phase and does not reproduce the metal‐to‐insulator transition of VO2 correctly, even with modified values of Ueff. On the other hand, sc‐PBE0 and SCAN describe the relative stability and the electronic structure of both polymorphs correctly and also provide reasonable lattice parameters. The functional SCAN yields the optimal balance between computational efficiency and accuracy. © 2019 The Authors. Journal of Computational Chemistry published by Wiley Periodicals, Inc.

中文翻译:

用于预测二氧化钒特性的 DFT + U 方法的关键评估

在之前的一项研究 (Stahl 和 Bredow, Chem. Phys. Lett. 2018, 695, 28-33) 中,我们研究了两种二氧化钒 VO2 多晶型物的结构、能量和电子特性,它们具有改进的全局和范围分离的混合功能。由于混合方法在计算上要求很高,因此我们在本研究中评估了计算效率更高的 DFT + U 方法。我们评估了广泛使用的 Dudarev PBE + U 方法,其有效哈伯德参数 Ueff = 3.4 eV 的文献值。我们将两种 VO2 多晶型物的 PBE + U 结果与我们之前的结果、自洽的混合功能 sc-PBE0 和元 GGA 功能 SCAN 进行了比较。发现 PBE + U 方法产生强烈扭曲的单斜晶相并且不能正确再现 VO2 的金属到绝缘体的转变,即使修改了 Ueff 值也是如此。另一方面,sc-PBE0 和 SCAN 正确描述了两种多晶型物的相对稳定性和电子结构,并提供了合理的晶格参数。功能 SCAN 产生计算效率和准确性之间的最佳平衡。© 2019 作者。Wiley Periodicals, Inc. 出版的《计算化学杂志》。
更新日期:2019-11-11
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