In this work, we only considered static 2D IR spectra that were calculated for a single molecular structure. When extending the presented approach to the dynamical case, it will become necessary to consider a large number of additional structures. As any quantum-chemical approach will quickly become infeasible for larger systems and when considering thousands of structural snapshots from molecular dynamics simulations, this usually requires the use of empirically parametrized vibrational exciton models. However, as we have demonstrated L-VSCF/L-VCI also provides access to all the parameters required for the construction of such models. The local-mode anharmonic energy levels can be extracted from the L-VSCF calculation, whereas the harmonic coupling constants as well as the local-mode transition dipole moments are available from the harmonic frequency calculation in combination with the localization of the normal modes. This can be used as basis for the parametrization of vibrational exciton models, which we will also explore in our future work in order to enable the quantum-chemical prediction of 2D IR spectra of dynamical systems.