Here, we propose that the extended amide III region (between ca. 1200 and 1400 cm -1 ) should be another promising target for 2D-IR spectroscopy, and predict that the cross-peaks in this region will be highly sensitive to the secondary structure. This suggestion is backed up by our recently developed methodology for the efficient quantum-chemical calculation of 2D-IR spectra, which allows for the prediction of 2D-IR spectra for arbitrary molecular systems in any spectral region, without the need for an empirical parametrization.