Temperature-dependent dynamics of endohedral fullerene Sc2@C80(CH2Ph) studied by EPR spectroscopy.

Endohedral fullerenes are promising materials for the quantum information and quantum processing due to the unique properties of the electron-nuclear spin system well isolated from the environment inside the fullerene cage. The endofullerene Sc2@C80(CH2Ph) features a strong hyperfine interaction between one electron spin 1/2 localized at the Sc2 dimer and two equivalent 45Sc nuclear spins 7/2, which yields 64 well resolved EPR transitions. We report a comprehensive analysis of the temperature dependence of the EPR spectrum of Sc2@C80(CH2Ph) dissolved in d-toluene measured in a wide temperature range above and below the melting point. The nature of the electron spin coherence phase memory is investigated. The properties of all resonance lines in a liquid phase were treated within the model of the free rotational diffusion. Both, analytical expressions and numerical examination provide an excellent agreement between the experimental and simulated spectra. A detailed study of the experimental data confirms the assumption of the independent motions of the fullerene cage and the Sc2 core. The data obtained show three regimes of molecular motion detected at different temperatures: the free rotation of both the fullerene cage and its bi-metal core, the motion of the core in the frozen fullerene cage, and, finally, a state with a fixed structure of both parts of the metallofullerene molecules. The data analysis reveals a significant nuclear quadrupole interaction playing an important role for the mixing of the different nuclear spin multiplets.