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

Timmers, Henry; Zhu, Xiaolei; Li, Zheng; Kobayashi, Yuki; Sabbar, Mazyar; Hollstein, Maximilian; Reduzzi, Maurizio; Martínez, Todd J.; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1038/s41467-019-10789-7

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

Journal Article · Tue Jul 16 00:00:00 EDT 2019 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-10789-7· OSTI ID:1546796

Timmers, Henry ^[1];

^[2];

^[3];

^[1]; Sabbar, Mazyar ^[1]; Hollstein, Maximilian ^[4]; Reduzzi, Maurizio ^[1];

^[2];

^[5]; Leone, Stephen R. ^[1]

Univ. of California, Berkeley, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Max Planck Inst. for the Structure and Dynamics of Matter, Hamburg (Germany); Peking Univ., Beijing (China)
Univ. of Hamburg (Germany)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

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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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); Army Research Office (ARO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC02-76SF00515; W911NF-14-1-0383; CHE-1361226; CHE-1660417; AC02-05CH11231

OSTI ID:: 1546796

Alternate ID(s):: OSTI ID: 1559236

Journal Information:: Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 45 works

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