Department of Chemistry, University of Western Ontario, London, Ontario N6A 5B7, Canada.
J Chem Phys. 2012 May 21;136(19):194501. doi: 10.1063/1.4716180.
We report a resonant inelastic x-ray scattering (RIXS) study of crystalline CeB(6). Ce L(α1,2) RIXS was measured with excitation energies resonant with the Ce L(3)-edge. A lifetime-broadening suppressed x-ray absorption near-edge structure (LBS-XANES), which successfully reproduced the L(α1,2) RIXS spectra over wide ranges of excitation and emission energies, was simulated using the SIM-RIXS program. A pre-edge structure in the LBS-XANES can be resolved, and many-body effects were suggested in the L(α1,2) RIXS around the Ce L(3)-edge energy. No convincing signs of Ce (II) or Ce (IV) states were observed in the LBS-XANES. Ce L(γ4) RIXS was measured at 302 K and 28 K with excitation energies across the Ce L(1)-edge. The interactions of p-valence electrons between Ce and B(6) were found to be considerably small, regardless of temperature. Thus, the electronic state of CeB(6) was concluded to be suitably described as a nominally Ce(4f(1))(3+)(e(-))(B(6))(2-) system with some hybridization among all valence orbitals of Ce and B.
我们报告了对 CeB(6)晶体的共振非弹性 X 射线散射(RIXS)研究。Ce L(α1,2) RIXS 是在与 Ce L(3)边缘共振的激发能下测量的。使用 SIM-RIXS 程序模拟了寿命展宽抑制的 X 射线吸收近边缘结构(LBS-XANES),该结构成功地在宽激发和发射能量范围内再现了 L(α1,2) RIXS 光谱。LBS-XANES 中可以分辨出预边结构,并且在 Ce L(3)边缘能量周围的 L(α1,2) RIXS 中存在多体效应。在 LBS-XANES 中未观察到 Ce(II)或 Ce(IV)态的明显迹象。在 302 K 和 28 K 下测量了 Ce L(γ4) RIXS,激发能横跨 Ce L(1)边缘。无论温度如何,Ce 和 B(6)之间的 p 价电子相互作用都被发现相当小。因此,CeB(6)的电子态被认为可以适当地描述为具有一定程度杂化的 Ce(4f(1))(3+)(e(-))(B(6))(2-)系统。