Abstract

Abstract We have theoretically investigated two-dimensional vibrational spectra for a two-mode system in terms of a diagrammatic approach. The two vibrational modes are anharmonically coupled. The perturbed stationary states are obtained by treating the cubic anharmonicity as a perturbation, and expressions for the third order response functions are derived. A physical origin of cross peaks in the spectrum is discussed. It is found that the vibrational dephasing time as well as the anharmonicity is important for the appearance of cross peaks.

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