Transient optical Kerr effect of liquids C2H4Cl2 and C2H4Br2 is investigated, for the first time to our knowledge, with a femtosecond (fs) probe laser delayed with respect to a coherent fs pump laser. Coherent coupling and electronic Kerr signals are observed around zero delay when pump and probe overlap. Persisting after the pump-probe overlap are Kerr signals arising from the torsional and other intramolecular vibrations of the trans and gauche conformations; Kerr signals arising from the intermolecular motion are also observed. Vibrational quantum interference is only observed in liquid C2H4Br2 and the related beats data are fitted with the torsional vibrations, 91 cm-1 (gauche) and 132 cm-1 (trans), and the CCBr angle-bending vibrations, 231 cm-1 (gauche) and 190 cm-1 (trans), with dephasing times, 0.45 ps, 0.45 ps, 2 ps, and 1.5 ps, respectively. These vibrational frequencies agree with those obtained in the frequency-domain. That no vibrational mode is observed for C2H4Cl2 might be attributed to ineffective Raman-pumping. Kerr signals observed after the pump-probe overlap are Fourier transformed to give the spectra of the intermolecular motion and the vibrational spectrum, which agrees with the one observed in the infrared absorption and/or Raman scattering heretofore.
- 1,2-dihaloethane liquids
- Femtosecond laser
- Raman-induced optical Kerr effect
- Vibrational spectroscopy