摘要
Understanding the evolution of molecular electronic structures is the key to explore and control photochemical reactions and photobiological processes.Subjected to strong laser fields,electronic holes are formed upon ionization and evolve in the attosecond timescale.It is crucial to probe the electronic dynamics in real time with attosecond-temporal and atomic-spatial precision.Here,we present molecular attosecond interferometry that enables the in situ manipulation of holes in carbon dioxide molecules via the interferometry of the phase-locked electrons(propagating in opposite directions)of a laser-triggered rotational wave packet.The joint measurement on high-harmonic and terahertz spectroscopy(HATS)provides a unique tool for understanding electron dynamics from picoseconds to attoseconds.The optimum phases of two-color pulses for controlling the electron wave packet are precisely determined owing to the robust reference provided with the terahertz pulse generation.It is noteworthy that the contribution of HOMO-1 and HOMO-2 increases reflecting the deformation of the hole as the harmonic order increases.Our method can be applied to study hole dynamics of complex molecules and electron correlations during the strong-field process.The threefold control through molecular alignment,laser polarization,and the two-color pulse phase delay allows the precise manipulation of the transient hole paving the way for new advances in attochemistry.
基金
supported by the National Key Research and Development Program of China(Grant Nos.2019YFA0307703,2019YFA0307700,and 2016YFA0401100)
the Major Research Plan of the National Natural Science Foundation of China(Grant No.91850201)
the National Natural Science Foundation of China(Grant Nos.11804388,11874066,11904400,U1830206,and 11974426).
