Molecular rovibrational dynamics investigated by two-photon wavepacket interferometry with phase-locked pulse pairs

Time-resolved two-photon fluorescence spectra have been investigated based on wavepacket interferometry (WPI), and the wavepacket dynamics of the excited states for 4-dicyanomethylene-2-methyl-6-p-dimethyl-aminostryryl-4H-pyran (DCM) is determined by phase-locked femtosecond pulse pairs. A relative phase between the femtosecond pulse pairs can be maintained as the delay line scanning, and so the two-photon fluorescence signals will be observed to appear periodically recurring features. It indicates the constructive or destructive interference between two-photon wavepackets on the molecular excited states. The experimental results show that the phase-locked WPI has the potential applications in the wavepacket dynamics of the complicated molecular systems.