基于第一性原理的氟氧化物结构和性质预测的交换相关函数性能评估
Assessing exchange-correlation functional performance for structure and property predictions of oxyfluoride compounds from first principles
摘要：
受有序氟化物和氟氧化物的电子和光学性质设计的复兴的启发，我们提出了一个密度泛函理论（DFT）研究19种材料的结构，从简单到复杂，和可变的氧氟比。我们专注于理解的准确性的交换相关势（$V_{xc}$）DFT预测的结构，电子和晶格动力学性质在四个不同的理论水平，\emph{i.e.}，局域密度近似（LDA），广义梯度近似（GGA），元GGA，和混合功能水平，其中包括分数的确切交换。我们详细研究了元GGA泛函MS 2 [Sun \emph{et al} .，物理学\修订版本\信件：\textbf{111}，106401（2013）]和SCAN [Sun \emph{et al} .，物理学\修订版本\信件：\textbf{115}，036402（2015）]，并且表明尽管元GGA在描述电子结构和声子频率方面显示出对LDA和GGA泛函的改进，但是氟化物和氟氧化物的静态结构性质通常由GGA级泛函PBesol更准确地预测。LDA计算的结果对于任何化合物都是不令人满意的，无论氧浓度如何。PBESol或HSE 06在所有氧化物或所有氟化物化合物中均具有良好的性能。对于氟氧化物，PBESol在所有氧浓度下的结构特性始终更准确，但是，我们强调需要对具有可变组成的氟氧化物进行详细的性能评估。“最佳”泛函预计将更强烈地依赖于感兴趣的属性。我们的研究提供了有用的见解，在选择一个$V_{xc}$，实现最佳的性能组成，使更准确的预测设计的功能性氟基材料与密度泛函理论。
英文摘要：
Motivated by the resurgence of electronic and optical property design in ordered fluoride and oxyfluoride compounds, we present a density functional theory (DFT) study on 19 materials with structures, ranging from simple to complex, and variable oxygen-to-fluorine ratios. We focus on understanding the accuracy of the exchange-correlation potentials ($V_{xc}$) to DFT for the prediction of structural, electronic, and lattice dynamical properties at four different levels of theory, \emph{i.e.}, the local density approximation (LDA), generalized gradient approximation (GGA), metaGGA, and hybrid functional level which includes fractions of exact exchange. We investigate in detail the metaGGA functionals MS2 [Sun \emph{et al}., Phys.\ Rev.\ Lett., \textbf{111}, 106401 (2013)] and SCAN [Sun \emph{et al}., Phys.\ Rev.\ Lett., \textbf{115}, 036402 (2015)], and show that although the metaGGAs show improvements over the LDA and GGA functionals in describing the electronic structure and phonon frequencies, the static structural properties of fluorides and oxyfluorides are often more accurately predicted by the GGA-level functional PBEsol. Results from LDA calculations are unsatisfactory for any compound regardless of oxygen concentration. PBEsol or HSE06 gives good performance in all oxide or all fluoride compounds. For the oxyfluorides, PBEsol is consistently more accurate for structural properties across all oxygen concentrations, however, we stress the need for detailed property assessment with various functionals for oxyfluorides with variable composition. The "best" functional is anticipated to be more strongly dependent on the property of interest. Our study provides useful insights in selecting an $V_{xc}$ that achieves the best performance comprise, enabling more accurate predictive design of functional fluoride-based materials with density functional theory.
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