NiO的2p3s3p, 2p3p3p和2p3s3s共振俄歇光谱

IF 9.3 2区 化学 Q1 CHEMISTRY, PHYSICAL
M. Finazzi, N. Brookes, F. Groot
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引用次数: 22

摘要

我们研究了NiO的2p3s3p、2p3p3p和2p3s3s俄歇线的行为,NiO是一种强相关三维体系中的模型化合物,同时改变了Ni L3和L2吸收边的光子能量。并将实验数据与基于电荷转移多重方法的理论模型进行了比较。当激发能低于L3共振时,我们观察到2p3p3p和2p3s3p的峰值处于恒定的结合能。这是典型的非辐射共振拉曼散射。如果光子能量进一步增大,2p3p3p和2p3s3p谱线迅速转化为恒定动能特征,呈现正常的俄歇行为。从拉曼行为到类俄歇行为的转变发生在光子能量低于对应于光电子激发到配空穴态的光子能量时。这可能表明在核心洞的重组中有非弹性过程的参与,涉及的能量远小于NiO间隙,或者可能存在非局部效应。在L3边缘的高光子能量侧,2p3p3p和2p3s3p峰的恒定动能系统地大于远高于L2,3边缘的激发所观察到的动能。我们将这种行为归因于2p^5 3d^10特征的中间态的干预,该特征的权重很小,但在共振时被强烈增强。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
2p3s3p, 2p3p3p, and 2p3s3s resonant Auger spectroscopy from NiO
We have investigated the behavior of the 2p3s3p, 2p3p3p, and 2p3s3s Auger lines of NiO, a model compound in the class of strongly correlated 3d systems, while varying the photon energy across the Ni L3 and L2 absorption edges. The experimental data are discussed in comparison with a theoretical model based on a charge-transfer multiplet approach. When the excitation energy is below the L3 resonance, we observe the 2p3p3p and 2p3s3p peaks at a constant binding energy. This behavior is typical of nonradiative resonant Raman scattering. If the photon energy is increased further, the 2p3p3p and 2p3s3p lines rapidly transform into constant kinetic energy features, showing a normal Auger behavior. The transition from Raman- to Auger-like behavior takes place for photon energies lower than the ones corresponding to excitations of the photoelectron into ligand-hole states. This might indicate the participation of inelastic processes in the recombination of the core hole involving energies much smaller than the NiO gap, or the possible presence of nonlocal effects. On the high photon energy side of the L3 edge, the constant kinetic energy of the 2p3p3p and 2p3s3p peaks is systematically larger than the one observed for an excitation well above the L2,3 edges. We attribute this behavior to the intervention of an intermediate state of 2p^5 3d^10 character, which has very little weight but is strongly enhanced at resonance.
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来源期刊
CiteScore
22.30
自引率
2.80%
发文量
29
期刊介绍: Catalysis Reviews is dedicated to fostering interdisciplinary perspectives in catalytic science and engineering, catering to a global audience of industrial and academic researchers. This journal serves as a bridge between the realms of heterogeneous, homogeneous, and bio-catalysis, providing a crucial and critical evaluation of the current state of catalytic science and engineering. Published topics encompass advances in technology and theory, engineering and chemical aspects of catalytic reactions, reactor design, computer models, analytical tools, and statistical evaluations.
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