Real-time observation of vibrational quantum beat in condensed phase by 20 fs time-resolved spectroscopy

Impulsive coherent vibrational spectroscopy is a kind of time-resolved spectroscopy methodology with a pulse duration of the femtosecond laser shorter than the molecular vibrational period. Usually, it is based on pump-probe technique and is utilized to real-time observation of the molecular vibrational dynamics coupled to the electronic ground or excited state. We have built an impulsive coherent vibrational spectroscopy setup based on a sub-20 fs, 550 to 700 nm tunable non-collinear optical parametric amplifier and performed pump-probe experiment with an Oxazine 720 methanol solution as the sample. Two vibrational quantum beats with frequency of 592 and 678 cm-1 were observed and the corresponding vibrational periods are 56.3 and 49.2 fs respectively.