For the amide I vibrations in polypeptides and proteins, which have been extensively studied in 2D-IR spectroscopy, such vibrational exciton models as well as the associated vibrational maps for modeling the required parameters, are well established and widely used for modeling 2D-IR spectra . The vibrational maps used in such simulations have been carefully constructed using quantum-chemical calculations for small model systems, such as N -methylacetamide (NMA) as well as dipeptides or by fitting to experimental data .