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

Timmers, H.; Zhu, X.; Li, Z.; Kobayashi, Y.; Sabbar, M.; Hollstein, M.; Reduzzi, M.; Martínez, T. J.; Neumark, D. M.; Leone, S. R.

doi:10.1038/s41467-019-10789-7

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

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Li, Z.
Department of Chemistry and The PULSE Institute, Stanford University;
SLAC Linear Accelerator Laboratory, Menlo Park;
International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Department of Physics, Peking University;

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Citation

Timmers, H., Zhu, X., Li, Z., Kobayashi, Y., Sabbar, M., Hollstein, M., et al. (2019). Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy. Nature Communications, 10: 3133. doi:10.1038/s41467-019-10789-7.

Cite as: https://hdl.handle.net/21.11116/0000-0005-D5E3-A

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.