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Polarization dependence of the ac Stark effect in multiphoton transitions of diatomic molecules

J. Chem. Phys. 97, 26 (1992); doi:10.1063/1.463624

Issue Date: 1 July 1992

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Bertrand Girard, Greg O. Sitz, and Richard N. Zare
Department of Chemistry, Stanford University, Stanford, California 94305

Nicolas Billy and Jacques Vigué
Laboratoire de Spectroscopie Hertzienne de l'E.N.S., 24 rue Lhomond, 75231 Paris Cedex 05, France
The (2+2) resonance-enhanced multiphoton ionization (REMPI) of N2 via the a 1Pig(v=1,J) levels shows a strong dependence on the polarization of the laser beam causing this process. This behavior is attributed to the ac Stark effect produced by the near resonance of the N2 o<sub>3</sub><sup>1</sup>Piu(v=0,J) levels with the sum of the first three photons. The multiphoton transitions are broadened and asymmetric in appearance; one level is even split. The line profiles change markedly as the polarization of the laser beam is varied from linear to circular. A general theory is presented for the ac Stark effect in a diatomic molecule undergoing a multiphoton transition. When the sum of the photon energies is resonant with an allowed transition, a splitting of the line is observed (Autler–Townes effect). Off resonance, the magnetic sublevels are shifted by different amounts, causing the line profile to be broadened and distorted. This theoretical treatment is able to explain in a satisfactory manner the observed behavior of (2+2) REMPI of N2 via the a 1Pig–X 1Sigma<sup> + </sup><sub>g</sub> transition and the two-photon laser-induced fluorescence of CO via the A 1Pi–X 1Sigma+ transition. The Journal of Chemical Physics is copyrighted by The American Institute of Physics.
History: Received 20 December 1991; accepted 16 March 1992
Permalink: http://link.aip.org/link/?JCPSA6/97/26/1
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KEYWORDS and PACS

Keywords
PACS
  • 33.55.Be
    Molecular spectra and interactions of molecules with photons Optical activity and dichroism; magnetooptical and electrooptical spectra Zeeman and Stark effects
  • YEAR: 1992

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0021-9606 (print)   1089-7690 (online)
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