High Harmonic Generation in Sulfur Dioxide

ORAL

Abstract

We show results of high harmonic generation (HHG) on the triatomic molecule sulfur dioxide. This molecule is one of the simplest systems having a conical intersection (CI), a region of electron degeneracy in which the Born-Oppenheimer approximation breaks down. A CI of particular interest exists between the excited electronic $^{1}$B$_{1}$ and $^{1}$A$_{2}$ states in the sulfur dioxide molecule. This CI can be reached via a direct Frank-Condon transition from the electronic ground state. The ionization and recombination steps of HHG render HHG a sensitive probe of electronic structure. HHG thus allows us to monitor electronic symmetry changes within the CI region, which has been shown to contain contributions from multiple orbitals [McFarland et al. \textit{Science} 2008]. We spectrally resolve the high harmonics of the ground and excited states of sulfur dioxide to characterize the CI, paving the way for a more complete understanding of non-Born-Oppenheimer dynamics.

*We gratefully acknowledge support from the DOE, office of BES and an NDSEG fellowship (LSS).

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Authors

  • Limor S. Spector

    • Stanford University

  • Joseph Farrell

    • Stanford University
    • PULSE Institute at the SLAC National Accelerator Laboratory

  • Brian McFarland

    • Stanford University
    • PULSE Institute at the SLAC National Accelerator Laboratory

  • Philip Bucksbaum

    • SLAC National Accelerator Laboratory, Stanford University
    • PULSE Institute at the SLAC National Accelerator Laboratory
    • PULSE Stanford
    • PULSE Institute for Ultrafast Energy Science, SLAC National Accelerator Laboratory, Menlo Park, CA 94025

  • Markus Guehr

    • SLAC National Accelerator Laboratory