Real-Space Observation Of Far- And Near-Field-Induced Photolysis Of Molecular Oxygen On An Ag(110) Surface By Visible Light
JOURNAL OF CHEMICAL PHYSICS(2019)
摘要
Dissociation of molecular oxygen is an important elementary process in heterogeneous catalysis. Here, we report on a real-space observation of oxygen photolysis on the Ag(110) surface at 78 K by far- and near-field excitation in the ultraviolet-near-infrared range using a low-temperature scanning tunneling microscope (STM) combined with wavelength-tunable laser excitation. The photolysis of isolated oxygen molecules on the surface occurs even by visible light with the cross section of similar to 10(-19) cm(2). Time-dependent density functional theory calculations reveal optical absorption of the hybridized O-2-Ag(110) complex in the visible and the near-infrared range which is associated with the oxygen photolysis. We suggest that the photolysis mechanism involves a direct charge transfer process. We also demonstrate that the photolysis can be largely enhanced in plasmonic STM junctions, and the cross section is estimated to be similar to 10(-17) cm(-2) in the visible and the near-infrared range, which appears to be an interesting feature of plasmon-induced reactions from the perspective of photochemical conversion with the aid of solar energy. Published under license by AIP Publishing.
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