Pulse-Train Photoelectron Spectroscopy of Electronic and Nuclear Dynamics in Molecules

Authors

  • Dr. Yasuki Arasaki,

    1. Department of Basic Science, Graduate School of Arts and Sciences, The University of Tokyo, Komaba, 153-8902, Tokyo (Japan)
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  • Prof. Dr. Kazuo Takatsuka

    Corresponding author
    1. Department of Basic Science, Graduate School of Arts and Sciences, The University of Tokyo, Komaba, 153-8902, Tokyo (Japan)
    • Department of Basic Science, Graduate School of Arts and Sciences, The University of Tokyo, Komaba, 153-8902, Tokyo (Japan)
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Abstract

We theoretically study the application of a femtosecond pulse train to simultaneously probe the electronic excitation dynamics and nuclear vibrational motion in the excited-state LiH molecule by means of time-resolved photoelectron spectroscopy. The step-like population transfers caused by continual interaction with a sequence of pulses and refractory periods are shown to give rise to time evolution of the photoelectron kinetic energy distribution as the history of molecular electronic and vibrational states. Such a signal should lead to a novel and direct way to investigate electronic and nuclear simultaneous dynamics involving multiple excited states.

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