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

Henry Timmers, Xiaolei Zhu, Zheng Li, Yuki Kobayashi, Mazyar Sabbar, Maximilian Hollstein, Maurizio Reduzzi, Todd J. Martínez, Daniel M. Neumark and Stephen R. Leone ()
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Henry Timmers: University of California
Xiaolei Zhu: Stanford University
Zheng Li: Stanford 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
Daniel M. Neumark: University of California
Stephen R. Leone: University of California

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-10789-7

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