Effect of Oriented External Electric Field in Altering Magnetic Exchange and Magnetic Anisotropy in Lanthanide‐Radical Complexes

Magnetic exchange coupling (J) is one of the important spin Hamiltonian parameters that control the magnetic characteristics of single-molecule magnets (SMMs). While numerous chemical methodologies have been proposed to modify ligands and control the J value, and magneto-structural correlations have been developed accordingly, altering this parameter through non-chemical means remains a challenging task. This study explores the impact of an Oriented-External Electric Field (OEEF) on over twenty lanthanide-radical complexes using Density Functional Theory (DFT) and ab initio Complete Active Space Self-Consistent Field (CASSCF) methods. Five complexes - [{(Me