We have tracked the behaviour of 102 distinct and identifiable vibrational couplings during the process of Myc2345 G-quadruplex folding, using EVV 2DIR spectroscopy, by titrating these features as a function of potassium ion concentration. The initial 102 peaks are modulated during folding in a number of ways including changes in intensity and frequency shifts plus the formation of two new and additional coupling peaks. Assignments of spectral features and explanations for the cause of changes to spectral features have been made with the aid of quantum-chemical (density functional theory) vibrational analysis and calculations of 2DIR spectra. Altogether, we find that there is evidence to suggest that Myc2345 forms unstacked G-quartet-resembling structures in the absence of ions, and that a different structure, presumed to be a G-quadruplex, forms upon potassium ion addition. More generally our work demonstrates that it is possible to obtain and interpret details about short range couplings even in the absence of long-range order. Secondly, it shows that a high density of interpretable features can be obtained using EVV 2DIR spectroscopy with high fidelity.