The folding of G4 from a relatively disordered to a relatively ordered structure would be expected to produce a few new coupling peaks as chemical groups previously separated are brought closer together. Figures and present the raw and fitted 2DIR spectra in the region of the observed new peaks 101 (𝜔 𝛼 = 1705 cm -1 , 𝜔 𝛽 -𝜔 𝛼 = 1675 cm -1 ) and 92 (𝜔 𝛼 = 1691 cm -1 , 𝜔 𝛽 -𝜔 𝛼 = 1132 cm -1 ), respectively. Figure presents the intensityion concentration dependence of both peaks. New vibrational modes extending over multiple Gquartets, and therefore having greater levels of delocalisation, can also result in the appearance of new peaks. These peaks may serve as markers of G4 formation. Assignments of these peaks will be discussed in the Discussion section.