Authors: Henry Timmers, Xiaolei Zhu, Zheng Li, Yuki Kobayashi, Mazyar Sabbar, Maximilian Hollstein, Maurizio Reduzzi, Todd J. Martínez, Daniel M. Neumark, Stephen R. Leone
Published: 2019-07-16
DOI: 10.1038/s41467-019-10789-7
Source: Full article
AbstractAttosecond 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.