State-resolved study of coadsorption effects on the stimulated dissociation of NO2on Pt(111)

A. R. Burns, T. M. Orlando, D. R. Jennison, Ellen Stechel

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

Stimulated surface processes, which are induced by electronic transitions, are especially sensitive to the presence of coadsorbates. We present here a detailed study of electron (5–350 eV) stimulated dissociation of chemisorbed NO2 on an O-covered Pt (111) surface, utilizing state-resolved laser resonance-ionization detection of the NO gas-phase product. Several dramatic effects on NO2 dissociation occur with increasing O atom coverage (up to θ 0 = 0.75 monolayer). First there is a large (X26) enhancement in the specific dissociation yield. Second, there is a narrowing of the translational energy distributions. A third observation is a distinct propensity (> 4:1 at low J) for populating the upper (Ω = 3/2) over the lower (Ω = 1/2) level of the spin-orbit-splitNO 2II Ω ground state. The enhanced yield can be understood in terms of increased lifetime(s) due to an O-induced reduction in charge transfer screening. Diminished charge transfer also reduces the vibrational and rotational excitation of the NO product. The spin-orbit propensity might arise from substrate reneutralization of NO+ following Auger decay of the primary excitation.

Original languageEnglish
Pages (from-to)1774-1778
Number of pages5
JournalJournal of Vacuum Science and Technology A: Vacuum, Surfaces and Films
Volume9
Issue number3
DOIs
Publication statusPublished - 1991

Fingerprint

dissociation
Charge transfer
Orbits
charge transfer
orbits
Surface states
products
Ground state
excitation
Ionization
Monolayers
Screening
energy distribution
screening
Gases
vapor phases
ionization
life (durability)
Atoms
ground state

ASJC Scopus subject areas

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

Cite this

State-resolved study of coadsorption effects on the stimulated dissociation of NO2on Pt(111). / Burns, A. R.; Orlando, T. M.; Jennison, D. R.; Stechel, Ellen.

In: Journal of Vacuum Science and Technology A: Vacuum, Surfaces and Films, Vol. 9, No. 3, 1991, p. 1774-1778.

Research output: Contribution to journalArticle

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AU - Stechel, Ellen

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N2 - Stimulated surface processes, which are induced by electronic transitions, are especially sensitive to the presence of coadsorbates. We present here a detailed study of electron (5–350 eV) stimulated dissociation of chemisorbed NO2 on an O-covered Pt (111) surface, utilizing state-resolved laser resonance-ionization detection of the NO gas-phase product. Several dramatic effects on NO2 dissociation occur with increasing O atom coverage (up to θ 0 = 0.75 monolayer). First there is a large (X26) enhancement in the specific dissociation yield. Second, there is a narrowing of the translational energy distributions. A third observation is a distinct propensity (> 4:1 at low J) for populating the upper (Ω = 3/2) over the lower (Ω = 1/2) level of the spin-orbit-splitNO 2II Ω ground state. The enhanced yield can be understood in terms of increased lifetime(s) due to an O-induced reduction in charge transfer screening. Diminished charge transfer also reduces the vibrational and rotational excitation of the NO product. The spin-orbit propensity might arise from substrate reneutralization of NO+ following Auger decay of the primary excitation.

AB - Stimulated surface processes, which are induced by electronic transitions, are especially sensitive to the presence of coadsorbates. We present here a detailed study of electron (5–350 eV) stimulated dissociation of chemisorbed NO2 on an O-covered Pt (111) surface, utilizing state-resolved laser resonance-ionization detection of the NO gas-phase product. Several dramatic effects on NO2 dissociation occur with increasing O atom coverage (up to θ 0 = 0.75 monolayer). First there is a large (X26) enhancement in the specific dissociation yield. Second, there is a narrowing of the translational energy distributions. A third observation is a distinct propensity (> 4:1 at low J) for populating the upper (Ω = 3/2) over the lower (Ω = 1/2) level of the spin-orbit-splitNO 2II Ω ground state. The enhanced yield can be understood in terms of increased lifetime(s) due to an O-induced reduction in charge transfer screening. Diminished charge transfer also reduces the vibrational and rotational excitation of the NO product. The spin-orbit propensity might arise from substrate reneutralization of NO+ following Auger decay of the primary excitation.

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