Orbital-resolved DFT+U for molecules and solids

We present an orbital-resolved extension of the Hubbard U correction to density-functional theory (DFT). Compared to the conventional shell-averaged approach, the prediction of energetic, electronic and structural properties is strongly improved, particularly for compounds characterized by both localized and hybridized states in the Hubbard manifold. The numerical values of all Hubbard parameters are readily obtained from linear-response calculations. The relevance of this more refined approach is showcased by its application to bulk solids pyrite (FeS₂) and pyrolusite (β-MnO₂), as well as to six Fe(II) molecular complexes. Our findings indicate that a careful definition of Hubbard manifolds is indispensable for extending the applicability of DFT+U beyond its current boundaries. The present orbital-resolved scheme aims to provide a computationally undemanding yet accurate tool for electronic structure calculations of charge-transfer insulators, transition-metal (TM) complexes and other compounds displaying significant orbital hybridization.
This dataset contains all Quantum ESPRESSO input and output files as well as all pseudopotentials that were used to generate the results of this study. Moreover, an ``EXAMPLES'' folder provides guidance on how to apply the LR-cDFT approach to evaluate orbital-resolved DFT+U parameters in practise.

我们提出了一种面向密度泛函理论（density-functional theory, DFT）的Hubbard U校正轨道分辨扩展方案。相较于传统壳层平均方法，该方案对能量、电子与结构性质的预测精度得到显著提升，尤其适用于Hubbard流形中同时存在局域态与杂化态的化合物。所有Hubbard参数的数值均可通过线性响应计算便捷获得。该更精细的方案的有效性，通过其在块体固体黄铁矿（FeS₂）、软锰矿（β-MnO₂）以及六种二价铁（Fe(II)）分子配合物中的应用得到验证。我们的研究结果表明，精准定义Hubbard流形对于将DFT+U的适用范围拓展至现有边界之外至关重要。本轨道分辨方案旨在为电荷转移绝缘体、过渡金属（transition-metal, TM）配合物以及其他存在显著轨道杂化的化合物的电子结构计算，提供一种计算成本低廉却精度可靠的工具。
本数据集包含本研究生成结果所用的全部Quantum ESPRESSO输入与输出文件，以及所有赝势文件。此外，「EXAMPLES」文件夹提供了实操应用线性响应校正密度泛函（LR-cDFT）方案以计算轨道分辨DFT+U参数的指导说明。