钴氧化物中位间4p-3d杂化的共振X射线发射光谱研究
Intersite 4p-3d hybridization in cobalt oxides: a resonant x-ray emission spectroscopy study
摘要：
我们报道了Co 1 s X射线吸收前沿中相邻Co原子到3d轨道的强偶极跃迁。它们揭示了通过应用高分辨率共振X射线发射光谱（RXES）的化合物含有CoO 6集群。当对比四极本地1 s3 d激发，这些非本地1 s3 d跃迁被确定由它们的能量色散和角度依赖性，它们的第二壳层效应的敏感性（即CoO 6八面体的连接模式和键长），和向上的能量移位2.5 eV由于较差的屏蔽的核心孔。实验表明，非局部跃迁的强度测量氧介导的4p-O-3d位点间杂交。我们提出了一个修正的解释过渡金属化合物的前边缘。对前边缘中这些新特征的详细分析提供了对过渡金属基系统中氧介导的金属-金属相互作用的独特见解，这是轨道有序和相关电子和磁性的关键方面。此外，本1 s2 p RXES实验的特殊分辨能力使我们能够证明底层散射过程的相干二阶性质。
英文摘要：
We report on strong dipole transitions to 3d orbitals of neighboring Co atoms in the Co 1s x-ray absorption pre-edge. They are revealed by applying high-resolution resonant x-ray emission spectroscopy (RXES) to compounds containing CoO6 clusters. When contrasted to quadrupole local 1s3d excitations, these non-local 1s3d transitions are identified by their energy dispersion and angular dependence, their sensitivity to second-shell effects (i.e. the connection mode of the CoO6 octahedra and the bond lengths), and an upwards energy shift of 2.5 eV due to the poorer screening of the core hole. The experiment reveals that the intensity of the non-local transitions gauges the oxygen-mediated 4p-O-3d intersite hybridization. We propose a revised interpretation of the pre-edges of transition metal compounds. Detailed analysis of these new features in the pre-edge offers a unique insight in the oxygen mediated metal-metal interactions in transition metal-based systems, which is a crucial aspect in orbital ordering and related electronic and magnetic properties. In addition, the exceptional resolving power of the present 1s2p RXES experiment allows us to demonstrate the coherent second-order nature of the underlying scattering process.
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