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The intense ultrashort laser pulse can be used to probe and control the rich electronic and nuclear dynamics of molecules using the multiphoton process. It is interesting not only for the fundamental optical molecular physics, but also for the coherent control of the chemical reactions. Experimentally, the electrons and ions ejected from a molecule are measured in coincidence with the cold target recoil ion momentum spectroscopy. In this talk, we show that the attosecond dynamics of electron localization can be directly probed and controlled from the diatomic to polyatomic hydrocarbon molecules, which is recently extended to two-dimensional stage. By coherently manipulating the rotational nuclear wave packet, we impulsively align and unidirectionally rotate the molecule to a terahertz frequency. We semi-classically trace and control the vibrational motion of the nuclei by using two time-delayed ultrashort laser pulses of detuned wavelengths. Our experiments furthermore reveal the electron-nuclear energy sharing in above-threshold multiphoton ionization of a molecule, which can be controlled by manipulating the molecular orientation. |
