Dephasing-induced vibronic resonances in difference frequency generation spectroscopy.
The difference frequency generation (DFG) signal from a two electronic level system with vibrational modes coupled to a Brownian oscillator bath is computed. Interference effects between two Liouville space pathways result in pure-dephasing-induced, excited-state resonances provided the two excitation pulses overlap and time ordering is not enforced. Numerical simulations of two-dimensional DFG signals illustrate how the ground and excited electronic state resonances may be distinguished.
Venkatramani
Ravindra
R
Department of Physics and Astronomy, University of Rochester, Rochester, New York 14627, USA.
Mukamel
Shaul
S
D002623:Chemistry Techniques, Analytical; D008956:Models, Chemical; D013057:Spectrum Analysis