Extended DFT+U method: application to analysis of complex doping effects, methodological developments and materials design.

去年，新提出的DFT+U方法的扩展，对具有相反自旋的电子之间的相互作用进行了修正（在标准DFT+U中不存在），已应用于过渡金属氧化物的形成能量和包含两种活性氧化还原中心的复杂电池阴极的电压分布的研究。详细的实验表明，利用新引入的修正项，使磁矩与实验值接近，可以计算出形成能。发现线性响应法对该任务不准确。此外，测试表明SCAN功能优于PBE。从而建立了过渡金属氧化物形成能的计算方法。对锰、铁、钒和铬氧化物进行了实验，得到的生成能和磁矩与实验结果吻合较好。扩展的DFT+U方法也被用于研究含有两种过渡金属（Ni和Mn）的层状氧化物结构的电化学性能。该方法对电压分布的预测非常准确，与实验结果吻合良好。对于标准DFT+U方法，也提出了一种鲁棒的U参数评估形式。

During the last year the newly proposed extension of DFT+U method with corrections for interactions between the electrons with opposite spins (absent in standard DFT+U) has been applied for the study of energies of formation of transition metal oxides and voltage profiles of complex battery cathodes that contain two types of active redox centers.Detailed tests revealed that energies of formation could be calculated by setting of magnetic moments close to experimental values by the newly introduced correction term. Linear response method was found not accurate for this task. Moreover tests have shown superiority of SCAN functional over PBE. Thus the methodology for evaluation of formation energies of transition metal oxides has been formulated. Tests have been performed for Mn, Fe, V and Cr oxides, yielding a good agreement with experiment for energies of formation and magnetic moments.The extended DFT+U method has been also applied for the study of electrochemical properties of a layered oxide structure, which contains two types of transition metals (Ni and Mn). This method provided very promising and accurate prediction of the voltage profile in a good agreement with experimental measurements. A robust form of evaluation of the U parameters has been proposed for the standard DFT+U method as well.