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Resonant core spectroscopies of the charge transfer interactions between C-60 and the surfaces of Au(111), Ag(111), Cu(111) and Pt(111)

机译:C-60与Au(111),Ag(111),Cu(111)和Pt(111)表面之间的电荷转移相互作用的共振核心光谱

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Charge transfer interactions between C-60 and the metal surfaces of Ag(111), Cu(111), Au(111) and Pt(111) have been studied using synchrotron-based photoemission, resonant photoemission and X-ray absorption spectroscopies. By placing the X-ray absorption and valence band spectra on a common binding energy scale, the energetic overlap of the unoccupied molecular orbitals with the density of states of the underlying metal surface have been assessed in the context of possible charge transfer pathways. Resonant photoemission and resonant Auger data, measuring the valence region as a function of photon energy for C-60 adsorbed on Au(111) reveals three constant high kinetic energy features associated with Auger-like core-hole decay involving an electron transferred from the surface to the LUMO of the molecule and electrons from the three highest occupied molecular orbitals, respectively and in the presence of ultra-fast charge transfer of the originally photoexcited molecule to the surface. Data for the C-60/Ag(111) surface reveals an additional Auger-like feature arising from a core-hole decay process involving more than one electron transferred from the surface into the LUMO. An analysis of the relative abundance of these core-hole decay channels estimates that on average 2.4 +/- 0.3 electrons are transferred from the Ag(111) surface into the LUMO. A core-hole clock analysis has also been applied to assess the charge transfer coupling in the other direction, from the molecule to the Au(111) and Ag(111) surfaces. Resonant photoemission and resonant Auger data for C-60 molecules adsorbed on the Pt(111) and Cu(111) surfaces are shown to exhibit no super-Auger features, which is attributed to the strong modification of the unoccupied molecular orbitals arising from stronger chemical coupling of the molecule to the surface.
机译:使用基于同步加速器的光发射,共振光发射和X射线吸收光谱研究了C-60与Ag(111),Cu(111),Au(111)和Pt(111)的金属表面之间的电荷转移相互作用。通过将X射线吸收和价带谱置于共同的结合能尺度上,在可能的电荷转移途径的背景下,对未占据的分子轨道的高能重叠与下层金属表面的态密度进行了评估。共振光发射和共振俄歇数据,测量吸附在Au(111)上的C-60的化合价与光子能量的函数关系,揭示出三个恒定的高动能特征,与涉及从表面转移的电子的俄歇样核孔衰变有关在最初的光激发分子超快速电荷转移到表面的情况下,分别从三个最高占据分子轨道的分子和电子转移到LUMO和电子。 C-60 / Ag(111)表面的数据显示出一个附加的俄歇样特征,是由于芯孔衰变过程引起的,该过程涉及从表面转移到LUMO的多个电子。这些芯孔衰变通道的相对丰度的分析估计平均有2.4 +/- 0.3电子从Ag(111)表面转移到LUMO。核孔时钟分析也已应用于评估从分子到Au(111)和Ag(111)表面在另一个方向上的电荷转移耦合。吸附在Pt(111)和Cu(111)表面上的C-60分子的共振光发射和共振俄歇数据显示不具有超俄歇特征,这归因于强化学作用引起的未占据分子轨道的强烈修饰分子与表面的偶联。

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