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Theoretical Insights into Unexpected Molecular Core Level Shifts: Chemical and Surface Effects
The Journal of Physical Chemistry Letters ( IF 5.7 ) Pub Date : 2017-11-10 00:00:00 , DOI: 10.1021/acs.jpclett.7b02583
A. Sarasola 1, 2 , M. Abadía 3 , C. Rogero 2, 3 , A. Garcia-Lekue 2, 4
Affiliation  

A set of density-functional theory based tools is employed to elucidate the influence of chemical and surface-induced changes on the core level shifts of X-ray photoelectron spectroscopy experiments. The capabilities of our tools are demonstrated by analyzing the origin of an unpredicted component in the N 1s core level spectra of metal phthalocyanine molecules (in particular ZnPc) adsorbed on Cu(110). We address surface induced effects, such as splitting of the lowest unoccupied molecular orbital or local electrostatic effects, demonstrating that these cannot account for the huge core level shift measured experimentally. Our calculations also show that, when adsorbed at low temperatures, these molecules might capture hydrogen atoms from the surface, giving rise to hydrogenated molecular species and, consequently, to an extra component in the molecular core level spectra. Only upon annealing, and subsequent hydrogen release, would the molecules recover their nominal structural and electronic properties.

中文翻译:

意外的分子核心能级变化的理论见解:化学和表面效应

使用一组基于密度泛函理论的工具来阐明化学和表面诱导的变化对X射线光电子能谱实验的核心能级位移的影响。通过分析吸附在Cu(110)上的金属酞菁分子(特别是ZnPc)的N 1s核心能级谱中不可预测成分的起源,证明了我们工具的功能。我们研究了表面感应效应,例如分裂了最低的未占据分子轨道或局部静电效应,证明了这些不能解释实验测得的巨大核能级位移。我们的计算还表明,当在低温下吸附时,这些分子可能会从表面捕获氢原子,从而产生氢化的分子种类,因此,分子核心能级谱中的额外成分。仅在退火和随后的氢释放时,分子才能恢复其标称结构和电子性质。
更新日期:2017-11-11
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