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Probing the geometry dependence of molecular dimers with two-dimensional-vibronic spectroscopy.

Two-dimensional (2D) vibronic correlation spectra of molecular dimers are calculated, taking a single vibration in each monomer into account. Within the employed wave function approach, the coupling to a surrounding is included only phenomenologically. It is shown that this offers a straightforward understanding of the spectra. The influence of the relative orientation of the monomer transition dipole moments and the electronic coupling strength is investigated. Employing a model for perylene bisimide, we predict the 2D-vibronic spectra for the monomer and dimer configurations.