Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy
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.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Jul 16, 2019
- Source ID
- 10.1038/s41467-019-10789-7
Entities
People
- Daniel Neumark
- Henry Timmers
- Maurizio Reduzzi
- Maximilian Hollstein
- Mazyar Sabbar
- Stephen R. Leone
- Todd Martinez
- Xiaolei Zhu
- Yuki Kobayashi
- Zheng Li
Organizations
- Army Research Office
- National Science Foundation