Two-photon resonant second harmonic generation in atomic xeon

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Abstract

Vacuum ultraviolet (VUV) radiation at 124.8 nm (9.93 eV) was produced from two-photon resonant second harmonic generation (SHG) in a xeon gaseous medium and used to probe molecular samples of acetone, furan, thiophene, ammonia, and methane. The mass spectra recorded from the species with ionization energies below 9.93 eV were dominated by the parent ions. The parent ions were only observed when the incident UV radiation was tuned to resonate with the two-photon transition 5 p5 (2P03/2 0) 6p [1/2]0 ←5 p6 1S 0 of Xe at 80 119.474 cm-1. The pressure dependence and the resonant nature of the parent ions observed support the mechanism for SHG as the ionization-initiated electric field induced SHG via the third-order nonlinear susceptibility X (3), which is enhanced by the coupling between the 5 p5 (P2 3/20) 6p [1/2]0 and the nearby 5 p5 (P2 3/20) 5d [1/2]1 states of Xe atoms.

Original languageEnglish
Article number094305
JournalThe Journal of Chemical Physics
Volume130
Issue number9
DOIs
StatePublished - 2009
Externally publishedYes

Bibliographical note

Funding Information:
This work was supported by National Science and Engineering Research Council (NSERC) of Canada, the Canadian Foundation for Innovation (CFI, New Opportunities Fund), and the University of Calgary. Y. J. S. is grateful for a NSERC University Faculty Award.

ASJC Scopus subject areas

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry

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