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

Author

Listed:
  • Henry Timmers

    (University of California)

  • Xiaolei Zhu

    (Stanford University
    SLAC Linear Accelerator Laboratory)

  • Zheng Li

    (Stanford University
    SLAC Linear Accelerator Laboratory
    Max Planck Institute for the Structure and Dynamics of Matter
    Peking University)

  • Yuki Kobayashi

    (University of California)

  • Mazyar Sabbar

    (University of California)

  • Maximilian Hollstein

    (University of Hamburg)

  • Maurizio Reduzzi

    (University of California)

  • Todd J. Martínez

    (Stanford University
    SLAC Linear Accelerator Laboratory)

  • Daniel M. Neumark

    (University of California
    Lawrence Berkeley National Laboratory)

  • Stephen R. Leone

    (University of California
    Lawrence Berkeley National Laboratory
    University of California)

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.

Suggested Citation

  • Henry Timmers & Xiaolei Zhu & Zheng Li & Yuki Kobayashi & Mazyar Sabbar & Maximilian Hollstein & Maurizio Reduzzi & Todd J. Martínez & Daniel M. Neumark & Stephen R. Leone, 2019. "Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-10789-7
    DOI: 10.1038/s41467-019-10789-7
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