Imaging electronic excitation of NO by ultrafast laser tunneling ionization

T. Endo, A. Matsuda, M. Fushitani, T. Yasuike, O. I. Tolstikhin, T. Morishita and A. Hishikawa, Physical Review Letters, 2016 116, 163002
DOI: 10.1103/PhysRevLett.116.163002
  • Electron motion governs bond-breaking and bond-making between molecules. Shooting movies of electrons is thus a long-standing goal of physicists and chemists pursuing a deeper understanding of chemical reactions. Laser tunneling ionization is a promising approach towards this goal that requires a high temporal resolution in the femtosecond range or shorter. In fact, the laser tunneling ionization has been successfully applied to static imaging of ground-state molecules. On the other hand, the applicability to excited states is not trivial. This is because of their small ionization potentials, which may introduce significant contributions from multiphoton process (instead of tunneling) to the ionization. Supported by quantitative comparisons with solid theories, the present study demonstrates that the laser tunneling imaging can visualize the electron distribution in a short-lived, excited molecules and the change upon photoabsorption. The present study demonstrates the visualization of photoexcitation in a molecule - a model reaction involving electron rearrangement - by laser tunneling ionization, thus suggesting a route to shoot ultrafast electron movies during chemical reactions.

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