We report the results of Raman and synchrotron infrared absorption measurements of several molecular phases of solid nitrogen to pressures above 100 GPa (300 K). Low- temperature vibrational spectra to 45 GPa are also presented. The changes in Raman and infrared spectra at 60 GPa and 300 K are interpreted as arising from the ε→ ζ transition reported at low temperature. The character of splitting of the Raman vibron ν₂ observed at 25 GPa and low temperatures differs from that previously reported, a difference that we ascribe to different experimental procedures employed and metastability of the low- temperature phase.