Electronic Structure of the CO/Pt(111) Electrode Interface Probed by Potential-Dependent IR/Visible Double Resonance Sum Frequency Generation Spectroscopy
Electronic Structure of the CO/Pt(111) Electrode Interface Probed by Potential-Dependent IR/Visible Double Resonance Sum Frequency Generation Spectroscopy
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电位相关红外/可见光双共振和频发生光谱探测 CO/Pt(111) 电极界面的电子结构
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发表时间：
2015
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通讯作者：
K. Uosaki
中科院分区：
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作者：
Shuo Yang;H. Noguchi;K. Uosaki
为了解释CO阳极氧化前Pt（111）电极上预吸附CO伸缩引起的和频峰强度异常增加的原因，用8种不同的可见光（527 ~ 635 nm）进行了电位依赖的和频测量.在除527 nm外的所有可见光下观察到异常SFG强度峰，并且SFG峰的电势随可见光能量移动1 V/eV，表明SFG强度异常增加的原因不是由于吸附CO的几何结构变化，而是由于可见光和/或可见光的共振。结果表明，SFG光谱不仅可以探测分子结构，而且可以探测电化学界面的电子结构，而这是电化学界面的电子结构难以确定的。
To clarify the origin of the anomalous increase of the intensity of the sum frequency generation (SFG) peak corresponding to the stretching of preadsorbed CO on a Pt(111) electrode in H2SO4 solution prior to anodic oxidation CO, potential-dependent SFG measurements were carried out by using eight different visible-light energies (527∼635 nm). Anomalous SFG intensity peaks were observed at all visible light except at 527 nm, and the potential of the SFG peak shifted with the visible-light energy by 1 V/eV, showing that the origin of the anomalous increase of SFG intensity is not due to the potential-dependent geometric structure change of adsorbed CO suggested before but due to a resonance of visible and/or SF light with electronic transition from the Fermi level of Pt(111) to the 5σa antibonding state of adsorbed CO. The present work showed that SFG spectroscopy can probe not only the molecular structure but also the electronic structure of the electrochemical interface, which is difficult to be determine...