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

在过去的一年里，新提出的扩展的DFT U方法被应用于过渡金属氧化物的生成能和含有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。详细的测试表明，通过新引入的校正项，通过设置接近实验值的磁矩，可以计算生成能。线性响应法被发现对这项任务不准确。此外，测试还显示了扫描函数比PBE的优越性。从而形成了计算过渡金属氧化物生成能的方法。对Mn、Fe、V和Cr氧化物进行了测试，得到了与实验相一致的生成能和磁矩。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质。这种方法提供了非常有前景的和准确的电压分布的预测，与实验测量结果很好地一致。对于标准的DFT-U方法，也提出了一种稳健的U参数估计形式。

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.