This year it will be 60 years since the process of self-association of guanosine-5'-monophosphate (5'-GMP) and the formation of G-tetrads and G-quadruplexes was first described.1 Since then, the structure and dynamics of these agglomerates have been studied by a wide range of techniques, with NMR and X-ray diffraction being the most widely used. Given the possibility to measure in a natural aqueous environment and the relative flexibility of the experiment to study the effects of external conditions and changes in the composition of interacting substances, vibrational spectroscopy (and especially Raman spectroscopy) form a suitable link between methods limited to low concentration (UV and CD spectroscopy) and X-ray structural analyzes of crystals.