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

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

Fingerprint

Molecular oxygen
Photolysis
photolysis
far fields
near fields
oxygen
Oxygen
Infrared radiation
Microscopes
microscopes
Scanning
Laser tuning
Laser excitation
scanning
cross sections
solar energy
tunable lasers
Solar energy
Light absorption
Catalysis

All Science Journal Classification (ASJC) codes

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

Cite this

Real-space observation of far- and near-field-induced photolysis of molecular oxygen on an Ag(110) surface by visible light. / Lin, Chenfang; Ikeda, Kei; Shiota, Yoshihito; Yoshizawa, Kazunari; Kumagai, Takashi.

In: Journal of Chemical Physics, Vol. 151, No. 14, 144705, 14.10.2019.

Research output: Contribution to journalArticle

@article{f4ffc96043e8473f80fe233e26eeaf0a,
title = "Real-space observation of far- and near-field-induced photolysis of molecular oxygen on an Ag(110) surface by visible light",
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.",
author = "Chenfang Lin and Kei Ikeda and Yoshihito Shiota and Kazunari Yoshizawa and Takashi Kumagai",
year = "2019",
month = "10",
day = "14",
doi = "10.1063/1.5112158",
language = "English",
volume = "151",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "American Institute of Physics Publising LLC",
number = "14",

}

TY - JOUR

T1 - Real-space observation of far- and near-field-induced photolysis of molecular oxygen on an Ag(110) surface by visible light

AU - Lin, Chenfang

AU - Ikeda, Kei

AU - Shiota, Yoshihito

AU - Yoshizawa, Kazunari

AU - Kumagai, Takashi

PY - 2019/10/14

Y1 - 2019/10/14

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85073210932&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85073210932&partnerID=8YFLogxK

U2 - 10.1063/1.5112158

DO - 10.1063/1.5112158

M3 - Article

C2 - 31615227

AN - SCOPUS:85073210932

VL - 151

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 14

M1 - 144705

ER -