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Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy.

  • Author(s): Timmers, Henry
  • Zhu, Xiaolei
  • Li, Zheng
  • Kobayashi, Yuki
  • Sabbar, Mazyar
  • Hollstein, Maximilian
  • Reduzzi, Maurizio
  • Martínez, Todd J
  • Neumark, Daniel M
  • Leone, Stephen R
  • et al.
Abstract

Attosecond probing of core-level electronic transitions provides a sensitive tool for studying valence molecular dynamics with atomic, state, and charge specificity. In this report, we employ attosecond transient absorption spectroscopy to follow the valence dynamics of strong-field initiated processes in methyl bromide. By probing the 3d core-to-valence transition, we resolve the strong field excitation and ensuing fragmentation of the neutral σ* excited states of methyl bromide. The results provide a clear signature of the non-adiabatic passage of the excited state wavepacket through a conical intersection. We additionally observe competing, strong field initiated processes arising in both the ground state and ionized molecule corresponding to vibrational and spin-orbit motion, respectively. The demonstrated ability to resolve simultaneous dynamics with few-femtosecond resolution presents a clear path forward in the implementation of attosecond XUV spectroscopy as a general tool for probing competing and complex molecular phenomena with unmatched temporal resolution.

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