Ultrafast Femtosecond Dynamics and High-Resolution Spectroscopy of Molecular Cations

Abstract Our recent studies on ultrafast nuclear dynamics and high-resolution spectroscopy of isolated molecular ions in which intense few-cycle near-IR laser pulses are used are introduced. By the pump–probe measurements of the fragmentation processes of methanol cations, we investigate ultrafast hydrogen migration in methanol cation in the time domain and determine vibrational frequencies of methanol cations in the frequency domain by Fourier transform of the yields of parent and fragment ions. We further demonstrate that the rovibrational level energy separations of D2 and D 2 + can be determined with ultrahigh resolution by strong-field Fourier transform spectroscopy.