Dy ₂ Schiff Base Single Molecule Magnet Forming a Halogen Bonding Network: Experiment and Theory

Magnetic relaxation, mediated through molecular and lattice vibrations, is recognised as the next hurdle to overcome in terms of high‐performaning Single Molecule Magnets (SMMs). One strategy is to confine molecular and lattice vibrations through intra‐ and intermolecular interactions to modulate the phonon spectrum. Here, we report the use of halogen bonding to engineer the crystal lattice of a Dy 2 dimer [Dy 2 Cl 4 (Hopch‐Br) 2 ]·CCl 4 involving disordered lattice solvent. The strength of the resulting network has been estimated using quantum chemical calculations. The magnetic data were investigated with SQUID magnetometry, revealing antiferromagnetic interactions between the two Dy III ions as well as slow relaxation of magnetisation, with the results being in excellent agreement with ab‐initio calculations.