SFG study of unstable surface species by picosecond pump-probe method

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

Research output: Contribution to journalConference articlepeer-review

19 Citations (Scopus)

Abstract

We succeeded in identifying the intermediates in thermal decomposition reactions by utilizing the combination of an instantaneous temperature jump induced by the irradiation of picosecond laser pulses and the subsequent observation by time-resolved sum-frequency generation (TR-SFG) spectroscopy. The short-lived reactive intermediates in the decomposition of formate on NiO(111) and Ni(111) surfaces were identified. The irradiation of 1064 nm laser pulses caused the vibrational peak of the C-D stretching mode vCD of bidentate formate on NiO(111) to weaken and the vCD band of monodentate formate to appear. The result on Ni(111) showed the weakening of the vCD band of bridging formate and the appearance of the C double bond O stretching mode vC double bond O of monodentate formate. The spectral changes recovered on a 100 ps time scale but not fully above 400 K for the NiO(111) system and 320 K for the Ni(111) system, indicating the onset of thermal decomposition in the high-temperature period. The observations suggested that the formate in the stable bidentate/bridging configurations transformed to unstable monodentate formate prior to decomposition. Temperature- and time-dependent features indicated that the two types of formate were in equilibrium and the equilibrium shifted towards the monodentate form by the rapid laser-induced temperature jump of about 250-300 K.

Original languageEnglish
Pages (from-to)349-357
Number of pages9
JournalSurface Science
Volume427-428
DOIs
Publication statusPublished - Jun 1 1999
Externally publishedYes
EventProceedings of the 1998 9th International Conference on Vibrations at Surfaces (VAS9) - Kanagawa-ken, Jpn
Duration: Oct 12 1998Oct 16 1998

All Science Journal Classification (ASJC) codes

  • Condensed Matter Physics
  • Surfaces and Interfaces
  • Surfaces, Coatings and Films
  • Materials Chemistry

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