Journal of Physical Chemistry A, Vol.107, No.41, 8388-8395, 2003
Interference, dephasing, and coherent control in time-resolved frequency domain two-dimensional vibrational spectra
The amplitude level quantum interference between different coherence pathways in doubly vibrationally enhanced four wave mixing (DOVE-FWM) can be used to control the relative intensities of different features in the two-dimensional vibrational spectrum of CS2 in CH2BrCl. The relative intensity reflects the final state populations that are controlled by the FWM processes. Modeling of the time dependent frequency-domain 2D spectra shows how the interference between pathways and their relative dephasing rates are responsible for the ability to control the relative intensity changes.