Magnetic Anisotropy of Dysprosium Encapsulated Metallofullerene Molecules：A Theoretical Study

A series of metallofullerene single-ion magnets embedded with [DyO]+ and [DyO2]– fragments were designed to probe the magnetic anisotropies and magnetic relaxation mechanisms using complete-active-space self-consistent field (CASSCF) calculations. CASSCF calculations show that the fullerenes with the different diameters exert marginally varying influences on both of the quantum tunneling of magnetization and the energy level splitting, ultimately causing changes in the energy barriers. It is interesting to find that [DyO]+ encapsulated in the fullerenes of C80 behave as the best. For [DyO2]–, however, the largest C100 is preferable due to the largest O−Dy−O angle. If the O−Dy−O angle is increased to 180°, the energy barrier of [DyO2@C100]− would be the largest up to 4075.9 cm−1.