Coherent electronic-vibrational dynamics in deuterium bromide probed via attosecond transient absorption spectroscopy

Author(s): Kobayashi, Yuki; Chang, Kristina F; Poullain, Sonia Marggi; Scutelnic, Valeriu; Zeng, Tao; Neumark, Daniel M; Leone, Stephen R | Abstract: Ultrafast laser excitation can trigger multiplex coherent dynamics in molecules. Here, we report attosecond transient absorption experiments addressing simultaneous probing of electronic and vibrational dynamics in a prototype molecule, deuterium bromide (DBr), following its strong-field ionization. Electronic and vibrational coherences in the ionic X$^2\Pi_{3/2}$ and X$^2\Pi_{1/2}$ states are characterized in the Br-$3d$ core-level absorption spectra via quantum beats with 12.6-fs and 19.9-fs periodicities, respectively. Polarization scans reveal that the phase of the electronic quantum beats depends on the probe direction, experimentally showing that the coherent electronic motion corresponds to the oscillation of the hole density along the ionization-field direction. The vibrational quantum beats are found to maintain a relatively constant amplitude, whereas the electronic quantum beats exhibit a partial decrease in time. Quantum wave-packet simulations show that the decoherence effect from the vibrational motion is insignificant because of the parallel relation between the X$^2\Pi_{3/2}$ and X$^2\Pi_{1/2}$ potentials. A comparison between the DBr and HBr results suggests that rotation motion is responsible for the decoherence since it leads to initial alignment prepared by the strong-field ionization.