title: Quantum diffusion wave-function approach to two-dimensional vibronic spectroscopy.
abstract: We apply the quantum diffusion wavefunction approach to calculate vibronic two-dimensional (2D) spectra. As an example, we use a system consisting of two electronic states with harmonic oscillator potentials which are coupled to a bath and interact with three time-delayed laser pulses. The first- and second-order perturbative wave functions which enter into the expression for the third-order polarization are determined for a sufficient number of stochastic runs. The wave-packet approach, besides being an alternative technique to calculate the spectra, offers an intuitive insight into the dissipation dynamics and its relation to the 2D vibronic spectra.
authors.affiliation: Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Hubland Campus Nord, Emil-Fischer-Str. 42, 97074 Würzburg, Germany.
authors.forename: Johannes
authors.initials: J
authors.lastname: Wehner
authors.affiliation: Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Hubland Campus Nord, Emil-Fischer-Str. 42, 97074 Würzburg, Germany.
authors.forename: Mirjam
authors.initials: M
authors.lastname: Falge
authors.affiliation: Institut für Theoretische Physik, TU Dresden, 01062 Dresden, Germany.
authors.forename: Walter T
authors.initials: WT
authors.lastname: Strunz
authors.affiliation: Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Hubland Campus Nord, Emil-Fischer-Str. 42, 97074 Würzburg, Germany.
authors.forename: Volker
authors.initials: V
authors.lastname: Engel