Two-dimensional femtosecond vibrational spectroscopy of liquids

Tanimura, Yoshitaka; Mukamel, Shaul
December 1993
Journal of Chemical Physics;12/15/1993, Vol. 99 Issue 12, p9496
Academic Journal
The nonlinear optical response of liquids subjected to a series of N femtosecond laser pulses is calculated using a multimode harmonic model for nuclear motions, with nonlinear coupling to the radiation field through the coordinate dependence of the electronic polarizability. Using electronically off-resonant optical fields, this multidimensional spectroscopy is shown to provide direct information regarding the homogeneous or the inhomogeneous nature of the spectral density obtained from optical birefringence measurements. Complementary information can be obtained using infrared pulses where the multiple time correlation functions of the nuclear dipole moment (rather than the electronic polarizability) are being probed.


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