Interference Effects in Vibronic 2D-Spectra of Diatomic Molecules

Abstract

Abstract We theoretically study interference effects in two-dimensional (2D) vibronic spectra which arise from two electronically excited states taking part in the multi-photon process initiated by femtosecond laser pulses. Therefore, a model is employed which mimiques the situation encountered in many halogen and interhalogen molecules. There, upon excitation from the ground state, an excited bound state and a dissociative state exist which are close in energy. We demonstrate that the different pathways to final states which enter into the third-order polarization result in pronounced interference patterns in the 2D-spectra.