Tracking molecular structure deformation of nitrobenzene and its torsion-vibration coupling by intense pumping CARS

The structural deformation induced by intense laser field of liquid nitrobenzene(NB) molecule,a typical molecule with restricting internal rotation,is tracked by time- and frequency-resolved coherent anti-Stokes.Raman spectroscopy(CARS) technique with an intense pump laser.The CARS spectra of liquid NB show that the NO_2 torsional mode couples with the NO_2 symmetric stretching mode,and the NB molecule undergoes ultrafast structural deformation with a relaxation time of 265 fs.The frequency of NO_2 torsional mode in liquid NB(42 cm~(-1)) at room temperature is found from the sum and difference combination bands involving the NO_2 symmetric stretching mode and torsional mode in time- and frequency-resolved CARS spectra.     

Vibrational relaxation dynamics in transient grating spectroscopy studied by rate equations based on time-dependent correlation function

A modified model, a set of rate equations based on time-dependent correlation function, is used to study vibrational relaxation dynamics in transient grating spectroscopy. The dephasing, the population dynamics, and the vibrational coherence concerning two vibrational states are observed respectively in organic dye IR780 perchlorate molecules doped polyvinyl alcohol matrix. The result shows that in addition to the information concerning system-environment interac- tion and vibrational coherence, the vibrational energy transfer can be described by this modified model.