Tan Xin Liang, Hagiwara Kenta, Chen Ying-Jiun, Schusser Jakub, Cojocariu Iulia, Baranowski Daniel, Feyer Vitaliy, Minár Ján, Schneider Claus M, Tusche Christian
Peter Grünberg Institut (PGI-6), Forschungszentrum Jülich, 52425, Jülich, Germany.
Peter Grünberg Institut (PGI-6), Forschungszentrum Jülich, 52425, Jülich, Germany.
Ultramicroscopy. 2023 Nov;253:113820. doi: 10.1016/j.ultramic.2023.113820. Epub 2023 Jul 31.
Fermi surfaces of transition metals, which describe all thermodynamical and transport quantities of solids, often fail to be modeled by one-electron mean-field theory due to strong correlations among the valence electrons. In addition, relativistic spin-orbit coupling pronounced in heavier elements lifts the degeneracy of the energy bands and further modifies the Fermi surface. Palladium and rhodium, two 4d metals attributed to show significant spin-orbit coupling and electron correlations, are ideal for a systematic and fundamental study of the two fundamental physical phenomena and their interplay in the electronic structure. In this study, we explored the Fermi surface of the 4d noble metals palladium and rhodium obtained via high-resolution constant initial state momentum microscopy. The complete 3D-Fermi surfaces of palladium and rhodium were tomographically mapped using soft X-ray photon energies from 34 eV up to 660 eV. To fully capture the orbital angular momentum of states across the Fermi surface, the Fermi surface tomography was performed using p- and s- polarized light. Applicability and limitations of the nearly-free electron final state model in photoemission are discussed using a complex band structure model supported by experimental evidence. The significance of spin-orbit coupling and electron correlations across the Fermi surfaces will be discussed within the context of the photoemission results. State-of-the-art fully relativistic Korringa-Kohn-Rostoker (KKR) calculations within the one-step model of photoemission are used to support the experimental results.
过渡金属的费米面描述了固体的所有热力学和输运量,但由于价电子之间的强关联,单电子平均场理论常常无法对其进行建模。此外,较重元素中显著的相对论自旋轨道耦合消除了能带简并,进一步改变了费米面。钯和铑这两种4d金属表现出显著的自旋轨道耦合和电子关联,是对这两种基本物理现象及其在电子结构中的相互作用进行系统而基础研究的理想对象。在本研究中,我们通过高分辨率的恒定初态动量显微镜探索了4d贵金属钯和铑的费米面。利用34 eV至660 eV的软X射线光子能量对钯和铑的完整三维费米面进行了断层扫描映射。为了全面捕捉费米面上态的轨道角动量,使用p偏振光和s偏振光进行了费米面断层扫描。利用实验证据支持的复杂能带结构模型,讨论了近自由电子终态模型在光电子发射中的适用性和局限性。将在光电子发射结果的背景下讨论费米面上自旋轨道耦合和电子关联的重要性。采用光电子发射单步模型中的最新全相对论科林加-科恩-罗斯托克(KKR)计算来支持实验结果。