Real-space observation of far- and near-field-induced photolysis of molecular oxygen on an Ag(110) surface by visible light

Chenfang Lin, Kei Ikeda, Yoshihito Shiota, Kazunari Yoshizawa, Takashi Kumagai

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

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 ∼10-19 cm2. Time-dependent density functional theory calculations reveal optical absorption of the hybridized O2-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 ∼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.

Original languageEnglish
Article number144705
JournalJournal of Chemical Physics
Volume151
Issue number14
DOIs
Publication statusPublished - Oct 14 2019

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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