A Flexible Approach for Engineering Macrocyclic High Performance Pentagonal Bipyramidal Dy(III) Single-Ion Magnets

A strong uniaxial ligand field generated by the Ph3SiO^- ligand combined with the weak equatorial field of the macrocyclic ligand LN5, generates [DyIII(LN5)(Ph3SiO)2]+, a pentagonal bipyramidal Dy(III) Single-Molecule Magnet with a high anisotropy barrier of 1108 K, and hysteresis loops open up to 14 K. Based on our synthetic blueprint, we use ab initio calculations to predict changes to the macrocycle to increase the barrier to ~ 1800 K.