Quantum resolved studies of electron-stimulated reactions on adsorbate covered Pt(111) surfaces

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

Research output: Contribution to journalArticle

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Abstract

Using laser resonance-enhanced ionisation spectroscopy, we have studied electron (6-350 eV) stimulated dissociation of NO2 coadsorbed with up to 0.75 monolayer of atomic O on Pt(111). Several dramatic effects on NO2 dissociation occur due to the presence of O. There is a large ( × 26) enhancement in the specific dissociation yield, a narrowing of the NO translational energy distributions, and a distinct propensity ( > 4:1 at low J) for populating the upper Ω = 3 2 NO spin-orbit level over the Ω = 1 2 level. The spin-orbit state distribution of the O(3PJ) dissociation fragment is (5.0): (2.5): (1.0) for J = 2, 1 and 0, which is within experimental error of the statistical (T → ∞) 2J + 1 limit. The enhanced yield probably results from an increased excited state lifetime due to a reduction in substrate charge-transfer screening. We have also detected O(3PJ = 2,1,0) and NO X2 Π 3 2, 1 2(v = 5) above an electron (6-350 eV) beam irradiated Pt(111) surface containing coadsorbed O2 and NO at 90 K. We conclude that both O(3PJ) and NO(v = 5) are laser-induced photodissociation fragments of NO2 desorbates. The NO2 is probably the reaction product of a collision between an O atom (created by electron-stimulated dissociation of adsorbed O2) and an NO(a). We correlate the 10 eV NO2 production threshold with the dissociative ionization of the 3σg molecular bonding orbital of O2(a).

Original languageEnglish
Pages (from-to)477-484
Number of pages8
JournalNuclear Inst. and Methods in Physics Research, B
Volume58
Issue number3-4
DOIs
Publication statusPublished - Jun 2 1991

Fingerprint

Adsorbates
dissociation
Electrons
electrons
Ionization
Orbits
fragments
Photodissociation
orbits
ionization
Lasers
Reaction products
Excited states
reaction products
photodissociation
lasers
Charge transfer
Monolayers
Screening
energy distribution

ASJC Scopus subject areas

  • Surfaces, Coatings and Films
  • Instrumentation
  • Surfaces and Interfaces

Cite this

Quantum resolved studies of electron-stimulated reactions on adsorbate covered Pt(111) surfaces. / Orlando, T. M.; Burns, A. R.; Stechel, Ellen; Jennison, D. R.

In: Nuclear Inst. and Methods in Physics Research, B, Vol. 58, No. 3-4, 02.06.1991, p. 477-484.

Research output: Contribution to journalArticle

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AB - Using laser resonance-enhanced ionisation spectroscopy, we have studied electron (6-350 eV) stimulated dissociation of NO2 coadsorbed with up to 0.75 monolayer of atomic O on Pt(111). Several dramatic effects on NO2 dissociation occur due to the presence of O. There is a large ( × 26) enhancement in the specific dissociation yield, a narrowing of the NO translational energy distributions, and a distinct propensity ( > 4:1 at low J) for populating the upper Ω = 3 2 NO spin-orbit level over the Ω = 1 2 level. The spin-orbit state distribution of the O(3PJ) dissociation fragment is (5.0): (2.5): (1.0) for J = 2, 1 and 0, which is within experimental error of the statistical (T → ∞) 2J + 1 limit. The enhanced yield probably results from an increased excited state lifetime due to a reduction in substrate charge-transfer screening. We have also detected O(3PJ = 2,1,0) and NO X2 Π 3 2, 1 2(v = 5) above an electron (6-350 eV) beam irradiated Pt(111) surface containing coadsorbed O2 and NO at 90 K. We conclude that both O(3PJ) and NO(v = 5) are laser-induced photodissociation fragments of NO2 desorbates. The NO2 is probably the reaction product of a collision between an O atom (created by electron-stimulated dissociation of adsorbed O2) and an NO(a). We correlate the 10 eV NO2 production threshold with the dissociative ionization of the 3σg molecular bonding orbital of O2(a).

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