In vacuo G-quartet and G-quadruplex molecular structures were first prepared using PyMol and then optimized with Gaussian at the density functional theory (DFT) level of theory using the B3LYP functional , and using the 6-31G(d,p) basis set , employing the Int=UltraFine grid granularity parameter and SCF=VeryTight convergence criterion. The optimized G-quartet and G-quadruplex structures were subsequently used with Gaussian, employing the same level of theory and basis set as for the geometry optimization, to calculate harmonic vibrational normal mode frequencies 𝜔 𝑖 and the dipole moment and polarizability and the first-order normal-mode derivative of the dipole moment, using numerical differentiation with in-house scripts of the dipole moment, dipole moment first derivative, and polarizability calculated at normal-mode displaced geometries to obtain the derivatives described above for the EVV 2DIR spectral intensities. We assumed a harmonic regime for the vibrational energy levels with a uniform scaling parameter of 0.96 , thus resulting in no difference between the sum 𝜔 𝑖 + 𝜔 𝑗 of singly excited energy levels and the combination/overtone energy level 𝜔 𝑖+𝑗 involving the same normal mode indices. The resulting data was then processed using in-house scripts into two-dimensional spectral intensities, each peak being dressed with 2D Gaussian lineshapes with a linewidth of 20 cm -1 (FWHM), and subsequently rendered using the Matplotlib Python library.