COHERENT CONTROL OF MOLECULAR EXCITATIONS IN THE CONDENSED PHASE USING OPTICAL HETERODYNE DETECTED RAMAN INDUCED KERR EFFECT SPECTROSCOPY

We explore vibrational coherences in condensed phase molecules which are created by simple phase modulated femtosecond laser pulses. Experiments are performed using optical heterodyne detected Raman-induced Kerr effect spectroscopy, which independently detects the real (birefringence) and imaginary (dichroism) components of the third order molecular response. For an excitation pulse with a specific duration and phase modulation, we find the experimental signals arising from the transient birefringence and dichroism to be qualitatively different. The experimental results are interpreted using a wavepacket picture.