**Appendix A**

For several selected bonds, the stretching spectra of four nucleotides are shown below in Figure A1 for the low resolution calculations.

Each bond between atoms *i* and *j* includes the projection of the vectors *vi* and *vj* on the bond's *rij* vector. Investigated spectra for each bond are evaluated from velocity autocorrelations for *i* and *j* atoms and are shown in black and red in the figures. Since each atom participates in several bonds' vibrations, calculated spectra contain low amplitude bands of adjacent bonds. The valid frequency range is 100–2000 cm<sup>−</sup>1. The calculations of spectra were done for approximately 16 ps, with the time step equal to 0.2 fs, at 40 cm<sup>−</sup><sup>1</sup> resolution. The Tables of calculated vibrational bands for the four types of nucleotides and their bases are collected in Supplementary Materials.

**Figure A1.** Stretching spectra of adenine, guanine, thymine C(1)–C(2)–C(3) bonds for atoms in hexagonal ring of the base, C(13)–N(7) stretching frequencies of cytosine in the base-to-2-deoxyribose bond, see numbering in the inserted scheme of each base. Red and black colors mark the *i-j* bond from the *i* and *j* side. Atoms at the side of the bond are written after the bond: X-Y X.
