SFG spectroscopy of CO/Ni(111): UV pumping and the transient hot band transition of adsorbed CO

Athula Bandara, Satoru S. Kano, Ken Onda, Satoshi Katano, Jun Kubota, Kazunari Domen, Chiaki Hirose, Akihide Wada

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13 Citations (Scopus)

Abstract

A UV excitation by a picosecond pulse at 266 nm induced an unusual shoulder on the v CO = 1 ← 0 resonance peak of CO/Ni(111) monitored by sum-frequency generation (SFG) of visible and IR pulses. The observed line shape was reproduced by the use of a dipole-dipole interaction model with the coherent potential approximation (CPA) where the hot band transition with a population ratio of 0.3 to 0.7 (v = 1 to v = 0) was assumed. Neither the transition to the two-phonon bound state nor the coupling with the low-frequency phonon modes explained the observed changes. The shoulder appeared only during the UV excitation, which indicated that the electronically driven excitation, presumably by the hot electrons generated by the irradiation, dominated the process. As possible mechanisms, the involvement of an intermediate negative ion resonance state and/or the non-adiabatic coupling of electronic states with C-O stretching mode were considered.

Original languageEnglish
Pages (from-to)1125-1132
Number of pages8
JournalBulletin of the Chemical Society of Japan
Volume75
Issue number5
DOIs
Publication statusPublished - May 1 2002
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Chemistry(all)

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