In this research work, the temperature dependence (T<100 K) of the rotational and oscillatory (precessional) motion frequencies around the axis passing through the single exo-drilling C–C bond of carbon clusters Cₙ (n=1, 3), adsorbed on the dimer row of the Si(100)2×1 surface as part of the exofullerenes C20@Cn and C60@Cn, as well as in the absence of fullerene adsorption, was studied. The study was carried out using the molecular dynamics method and modeled in the open-source simulator LAMMPS.