Quantum diffusion wave-function approach to two-dimensional vibronic spectroscopy.

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.