Theoretical Prediction of the Magnetic Blocking Temperature of Dysprosium-Based Metallofullerene Single-Molecule Magnets

Five geometrically similar dysprosium-based endohedral metallofullerenes (Dy-EMF), single-molecule magnets, namely, DySc2N@C80-D5d, DySc2N@C90-D5h, DySc2N@C100-D5d, DySc2N@C110-D5h, and DySc2N@C120-D5d, are investigated using DFT and CASSCF methods. Energy decomposition analysis reveals that the interaction between the endohedral cluster and the cage is predominantly electrostatic and is weakened sequentially as the cage size increases. The ground states of these molecules are all stabilized as mJ |±15/2>, with magnetic reversal barriers ranging from 999.3 to 1209.0 cm-1 and blocking temperatures ranging from 14.1 and 15.2 K. As the size of the cage increases, the magnetic blocking temperatures and relaxation times generally decrease. These findings offer important insights for the design of high-performance EMF SMMs.