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J Phys Chem B. 2005 Apr 28;109(16):8132-43.

Dephasing-induced vibronic resonances in difference frequency generation spectroscopy.

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  • 1Department of Physics and Astronomy, University of Rochester, Rochester, New York 14627, USA.


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.

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