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High Resolution Phonon-assisted Quasi-resonance Fluorescence Spectroscopy
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Two-photon resonant second harmonic generation in atomic xeon.

Y J Shi1, W Al-Basheer, R I Thompson

  • 1Department of Chemistry, University of Calgary, Calgary, Alberta T2N 1N4, Canada. shiy@ucalgary.ca

The Journal of Chemical Physics
|March 12, 2009
PubMed
Summary
This summary is machine-generated.

Researchers generated vacuum ultraviolet (VUV) radiation using resonant second harmonic generation in xenon. This VUV light efficiently ionized molecules with low ionization energies, producing parent ions via a specific two-photon transition.

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Area of Science:

  • Atomic, Molecular, and Optical Physics
  • Chemical Physics
  • Spectroscopy

Background:

  • Vacuum ultraviolet (VUV) radiation is crucial for probing molecular electronic structures.
  • Second harmonic generation (SHG) is a nonlinear optical process for generating shorter wavelengths.
  • Resonant enhancement can significantly improve nonlinear optical processes.

Purpose of the Study:

  • To generate VUV radiation at 124.8 nm (9.93 eV) using two-photon resonant SHG in xenon.
  • To investigate the ionization of various molecular samples using the generated VUV radiation.
  • To elucidate the mechanism of SHG in xenon, particularly the role of resonant enhancement.

Main Methods:

  • Generation of VUV radiation via two-photon resonant SHG in a xenon gas medium.
  • Probing molecular samples including acetone, furan, thiophene, ammonia, and methane.
  • Analysis of mass spectra to identify parent ions and fragmentation patterns.

Main Results:

  • VUV radiation at 124.8 nm was successfully produced through resonant SHG in xenon.
  • Mass spectra of molecules with ionization energies below 9.93 eV were dominated by parent ions.
  • Parent ion observation was strictly dependent on tuning the VUV radiation to a specific two-photon resonance in xenon.
  • Observed pressure dependence and resonant behavior support an ionization-initiated electric field induced SHG mechanism via chi((3)).

Conclusions:

  • Two-photon resonant SHG in xenon is an effective method for generating VUV radiation for molecular ionization studies.
  • The observed parent ion dominance indicates efficient single-photon ionization at the VUV wavelength.
  • The mechanism involves third-order nonlinear susceptibility enhanced by resonant coupling between xenon electronic states.