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  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., 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.

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 Creators:
Timmers, H.1, Author
Zhu, X.2, 3, Author
Li, Z.2, 3, 4, 5, 6, Author           
Kobayashi, Y.1, Author
Sabbar, M.1, Author
Hollstein, M.7, Author
Reduzzi, M.1, Author
Martínez, T. J.2, 3, Author
Neumark, D. M.1, 8, Author
Leone, S. R.1, 8, 9, Author
Affiliations:
1Department of Chemistry, University of California, ou_persistent22              
2Department of Chemistry and The PULSE Institute, Stanford University, ou_persistent22              
3SLAC Linear Accelerator Laboratory, Menlo Park, ou_persistent22              
4International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266714              
5Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_persistent22              
6Department of Physics, Peking University, ou_persistent22              
7Department of Physics, University of Hamburg, ou_persistent22              
8Chemical Sciences Division, Lawrence Berkeley National Laboratory, ou_persistent22              
9Department of Physics, University of California, ou_persistent22              

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 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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Language(s): eng - English
 Dates: 2019-02-102019-05-232019-07-16
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41467-019-10789-7
 Degree: -

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Project name : H.T., Y.K., D.M.N., and S.R.L. were supported by the Army Research Office (ARO) (W911NF-14-1-0383). X.Z. and T.J.M. acknowledge support by the AMOS program within the Chemical Sciences, Geosciences and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy. M.S. and M.R. were supported by the National Science Foundation (NSF) (CHE-1361226 and CHE-1660417). Z.L. acknowledges partial financial support from the VW foundation through Peter Paul Ewald fellowship. Y.K. additionally acknowledges financial support from the Funai Overseas Scholarship. We would like to thank Andrew Attar and Aditi Bhattacherjee for their help in setting up a vacuum integrated liquid nitrogen trap for handling halogenated species as well as Stefan Pabst for his fruitful discussions on strong field excitation mechanisms. We would also like to thank Rolf Heilemann and Henrik Koch for their help in CVS-CC method.
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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 10 Sequence Number: 3133 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723