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arXiv 0909.0894cond-mat.mtrl-scicond-mat.str-el
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高分辨X射线吸收谱研究高Tc铜氧化物Cu K边的多重边前结构

Multiple pre-edge structures in Cu K-edge of high Tc cuprates revealed by high resolution x-ray absorption spectroscopy

C. Gougoussis, J. -P. Rueff, M. Calandra, M. d'Astuto, I. Jarrige, H. Ishii, A. Shukla, I. Yamada, M. Azuma, M. Takano

摘要:

利用高分辨X射线吸收谱和最新的电子结构计算,我们证明了高T $_c$铜氧化物的Cu K边的边前区是由标准X射线吸收谱中不可见的几个激发态组成的。我们详细考虑的情况下,钙$_{2-x}$ CuO $_2$ Cl $_2$和表明,许多前边缘激发(两个为c轴偏振,四个为面内偏振和面外入射X射线动量)是占主导地位的离位跃迁和intersite杂化。这表明了相关材料的前边缘的描述的方法超出了单网站模型的相关性。最后,我们显示的主边缘峰,这是最明显的偏振是沿c轴时,发生了加倍。这种倍增现象在以前的任何铜酸盐吸收数据中都没有发现,也不能通过第一性原理计算再现。我们认为这个峰是由于多体电荷转移激发引起的,而所有其他可见的远边结构都是单粒子起源的。我们的工作表明,以前的解释的Cu K边X射线吸收光谱在高T $_c$铜酸盐可以有益地重新考虑。

英文摘要:

Using high resolution x-ray absorption spectroscopy and state-of-the-art electronic structure calculations we demonstrate that the pre-edge region at the Cu K-edge of high T$_c$ cuprates is composed of several excitationsinvisible in standard X-ray absorption spectra. We consider in detail the case of Ca$_{2-x}$CuO$_2$Cl$_2$ and show that the many pre-edge excitations (two for c-axis polarization, four for in-plane polarization and out-of-plane incident X-ray momentum) are dominated by off-site transitions and intersite hybridization. This demonstrates the relevance of approaches beyond the single-site model for the description of the pre-edges of correlated materials. Finally, we show the occurrence of a doubling of the main edge peak that is most visible when the polarization is along the c-axis. This doubling, that has not been seen in any previous absorption data in cuprates, is not reproduced by first principles calculations. We suggest that this peak is due to many-body charge-transfer excitations, while all the other visible far-edge structures are single particle in origin. Our work indicates that previous interpretations of the Cu K-edge X-ray absorption spectra in high T$_c$ cuprates can be profitably reconsidered.

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