Woicik J C, Weiland C, Jaye C, Fischer D A, Rumaiz A K, Shirley E L, Kas J J, Rehr J J
Materials Measurement Science Division, Material Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, USA.
National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, USA.
Phys Rev B. 2020 Jun;101(24). doi: 10.1103/physrevb.101.245119.
First-principles, real-time-cumulant, and Bethe-Salpeter-equation calculations fully capture the detailed satellite structure that occurs in response to the sudden creation of the core hole in both photoemission and x-ray absorption spectra of the transition-metal compounds SrTiO and rutile TiO. Analysis of the excited-state, real-space charge-density fluctuations betrays the physical nature of these many electron excitations that are shown to reflect the materials' solid-state electronic structure and chemical bonding. This first-principles development of the cumulant-based core hole spectral function is generally applicable to other systems and should become a standard tool for all similar spectroscopic analysis going beyond the quasiparticle physics of the photoelectric effect.
第一性原理、实时累积量和贝叶斯-萨尔皮特方程计算充分捕捉了在过渡金属化合物SrTiO和金红石TiO₂的光电子能谱和X射线吸收光谱中，因核心空穴的突然产生而出现的详细卫星结构。对激发态实空间电荷密度涨落的分析揭示了这些多电子激发的物理本质，这些激发反映了材料的固态电子结构和化学键。基于累积量的核心空穴谱函数的这一第一性原理发展通常适用于其他系统，并且应该成为超越光电效应准粒子物理的所有类似光谱分析的标准工具。
