论文标题

ti〜1 $ s $ S $核心级光谱srtio $ _3 $和tio $ _2 $中的卫星

Satellites in the Ti~1$s$ core level spectra of SrTiO$_3$ and TiO$_2$

论文作者

Hariki, Atsushi, Higashi, Keisuke, Yamaguchi, Tatsuya, Li, Jiebin, Kalha, Curran, Mascheck, Manfred, Eriksson, Susanna K., Wiell, Tomas, de Groot, Frank M. F., Regoutz, Anna

论文摘要

光电子光谱法(PE)核心水平光谱中的卫星可以提供有关材料中电子结构和化学键的关键信息,尤其是在过渡金属氧化物中。本文探讨了Ti 1 $ S $和2 $ P $ core级光谱的卫星Srtio $ _3 $和TIO $ _2 $。通常,软X射线PE(SXP)探测Ti 2 $ p $核心水平;但是,由于其固有的旋转轨道分解(SOS),完全捕获卫星特征并不理想。在这里,硬X射线PES(haxpes)提供了对Ti 1 $ s $频谱的访问,这使我们能够在创建核心孔时研究内在的电荷响应,而无需SOS的并发症,并且具有良好的内在线宽。从理论上讲,实验光谱是通过两个杂质模型分析的,包括建立在局部密度近似(LDA)和动态平均场理论(DMFT)的Anderson杂质模型(AIM),以及常规的TIO $ _6 $群集模型。理论上的结果强调了明确包含高阶Ti-O电荷转移过程的重要性,而不是最近邻居Ti-O债券以模拟SRTIO $ _3 $和TIO $ _2 $的核心水平光谱。 LDA+DMFT提供的连续浴轨道的目标方法很好地表示实验光谱。至关重要的是,借助LDA+DMFT方法,本文提供了强大的处方,即如何在拟合核心水平光谱的分析中使用计算廉价群集模型。

Satellites in core level spectra of photoelectron spectroscopy (PES) can provide crucial information on the electronic structure and chemical bonding in materials, particular in transition metal oxides. This paper explores satellites of the Ti 1$s$ and 2$p$ core level spectra of SrTiO$_3$ and TiO$_2$. Conventionally, soft x-ray PES (SXPS) probes the Ti 2$p$ core level; however, it is not ideal to fully capture satellite features due to its inherent spin-orbit-splitting (SOS). Here, hard x-ray PES(HAXPES) provides access to the Ti 1$s$ spectrum instead, which allows us to study intrinsic charge responses upon core-hole creation without the complication from SOS and with favorable intrinsic linewidths. The experimental spectra are theoretically analyzed by two impurity models, including an Anderson impurity model (AIM) built on local density approximation (LDA) and dynamical mean-field theory (DMFT), and a conventional TiO$_6$ cluster model. The theoretical results emphasize the importance of explicit inclusion of higher-order Ti-O charge-transfer processes beyond the nearest-neighboring Ti-O bond to simulate the core level spectra of SrTiO$_3$ and TiO$_2$. The AIM approach with continuous bath orbitals provided by LDA+DMFT represents the experimental spectra well. Crucially, with the aid of the LDA+DMFT method, this paper provides a robust prescription of how to use the computationally cheap cluster model in fitting analyses of core level spectra.

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