发表机构
Osaka Metropolitan University; Tokyo Metropolitan University; Max Planck Institute for Chemical Physics of Solids; Shibaura Instutite of Technology; University of Tokyo; Institute for Solid State Physics, University of Tokyo; National Synchrotron Radiation Research Center; Waseda University（大阪公立大学; 东京都立大学; 马克斯·普朗克固体化学物理研究所; 芝浦工业大学; 东京大学; 东京大学固体物理研究所; 国家同步辐射研究中心; 早稻田大学）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究采用DFT+DMFT方法，明确了NiS₂和NiSe₂的电荷转移能更小、Ni局域磁矩降低等电子结构特征，阐明了其低能电子结构的演化机制。
AI 中文摘要
我们采用密度泛函理论结合动力学平均场理论（DFT+DMFT）研究NiS₂和NiSe₂的电子结构。通过优化双计数校正以重现实验价带光电子能谱，确定了DFT+DMFT框架下的真实电子结构；该模型还成功描述了NiS₂的Ni 2p芯能级光电子能谱和Ni L边X射线吸收谱，进一步验证了其有效性。结果显示，电荷转移能比此前假设的更小，导致配体向Ni发生显著电荷转移，Ni的局域磁矩降低。我们阐明了Ni上哈伯德带与硫族元素二聚体反键态的相对位置及相互作用，如何调控NiS₂₋ₓSeₓ系列低能电子结构的演化。
英文摘要
We investigate the electronic structures of NiS$_2$ and NiSe$_2$ using density functional theory combined with dynamical mean-field theory (DFT+DMFT). A realistic electronic structure within DFT+DMFT was determined by optimizing the double-counting correction to reproduce experimental valence-band photoemission spectra. The validity of the present model is further confirmed by its successful description of the Ni 2$p$ core-level photoemission and Ni $L$-edge x-ray absorption spectra of NiS$_2$. Our results reveal a smaller charge-transfer energy than previously assumed, resulting in substantial ligand-to-Ni charge transfer and a reduced Ni local moment. We clarify how the relative position and interaction between the Ni upper Hubbard band and the antibonding chalcogen-dimer states shape the evolution of the low-energy electronic structure across the NiS$_{2-x}$Se$_x$ series.
