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

扩展 DFT U 方法：应用于复杂掺杂效应分析、方法开发和材料设计。

• 批准号: 22K05019
• 负责人: Shishkin Maxim
• 金额: $ 2.25万
• 依托单位: Tokyo Institute of Technology
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (C)
• 财政年份: 2022
• 资助国家: 日本
• 起止时间: 2022-04-01 至 2025-03-31
• 项目状态: 未结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-22K05019/
• 关键词: DFT+U; redox potentials; opposite spins; doping effect; materials design

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.

在过去的一年中，新提出的DFT+U方法的扩展与具有相反自旋的电子之间的相互作用的校正，（标准DFT+U中不存在）应用于研究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合电池阴极的电压分布，详细的实验表明，通过设定磁矩接近通过新引入的校正项将实验值与实验值进行比较。发现线性响应方法对于该任务不准确。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，并将扩展的DFT+U方法应用于含两种过渡金属（Ni和Mn）的层状氧化物结构的电化学性质的研究。这种方法提供了非常有前途的和准确的预测的电压分布与实验测量的良好协议。对于标准DFT+U方法，也提出了一种鲁棒的U参数评估形式。

项目成果

Layered Pt-Co alloys: bulk, surface and nanoparticle analysis, based on DFT

• DOI: 10.1016/j.susc.2022.122082
• 发表时间: 2022-03
• 期刊: Surface Science
• 影响因子: 1.9
• 作者: M. Shishkin;Takeo Yamaguchi