The conditions of the existence and the main characteristics (frequencies, intensities, and attenuation parameters) of discrete vibrational levels caused by structural defects of linear chains of inert gas atoms adsorbed on the surface of nanotubes aggregated in nanobundles, are calculated and analyzed. Discrete vibrational levels lying both above and below the band of the quasi-continuous spectrum of the chain are considered. Analytical expressions obtained for the frequencies of these discrete levels make it possible to determine with high precision the defect parameters (difference in the interaction with the substrate and with the atoms of the chain) basing on optical measurements.