In this paper, we report the use of a variant of 2DIR spectroscopy called Electron-Vibration-Vibration (EVV), which has the ability to measure across a wide spectral window and recover ~100 distinct and unique vibrational couplings for a typical protein or nucleic acid sample. EVV 2DIR spectroscopy, also known as DOVE FWM spectroscopy, was first demonstrated by Wright and Cho. It is a four-wave mixing technique in which two mid-IR pulses excite two vibrational states e.g., a fundamental vibration and a two-quantum combination state. A third non-resonant pulse using photon energies high enough for single photon counting, induces a Raman transition if the two excited modes are coupled and it is this Raman scattering which is detected as a homodyne signal. Since its inception, the technique has since been applied to the geometry determination of complexes, protein identification, quantification of tyrosine nitration in peptides, tissue imaging, and the detection of protein-ligand complexes. In this work we use EVV 2DIR spectroscopy in combination with quantum chemistry calculations based on density functional theory, to study the structural changes that occur in Myc2345 due to the addition of potassium ions, which shifts the position of thermodynamic equilibrium from an unfolded to a folded G4. The 22-mer DNA sequence Myc2345 forms an intramolecular, propeller-type, parallel-stranded G4 in the presence of potassium ions. The high intracellular concentration of K + ions suggests that K + -bound structures prevail under physiological conditions, which makes quadruplex conformations with K + of relevance.