Inducing magnetic coupling between 4f elements is an ongoing challenge.T oo vercome this formidable difficulty, we incorporate highly delocalized tetrazinyl radicals,w hich strongly couple with f-blockm etallocenes to form discrete tetranuclear complexes.S ynthesis,s tructure,a nd magnetic properties of two tetranuclear [(Cp* 2 Ln) 4 (tzC) 4 ]•3(C 6 H 6 ) (Cp* = pentamethylcyclopentadienyl;t z = 1,2,4,5-tetrazine; Ln = Dy,G d) complexes are reported. An in-depth examination of their magnetic properties through magnetic susceptibility measurements as well as computational studies support ah ighly sought-after radical-induced "giant-spin" model. Strong exchange interactions between the Ln III ions and tzC radicals lead to as trong magnet-like behaviour in this molecular magnet with alarge coercive field of 30 kOe.

The first example of unique coordination induced intramolecular pancake bonding was achieved through the reduction of two bis(pyrazolyl)-tetrazine ligands.

Tapping into the secondary coordination environment of mononuclear DyIII-complexes leads to drastic changes in luminescence and magnetism. Visualization of effects induced by stereoelectronics on the opto-magnetic properties was achieved through...

Magnetic coupling plays a critical role in the overall magnetic behaviour of a single-molecule magnet (SMM). Through a careful design strategy that employs the highly delocalized 1,2,4,5-tetrazinyl (tz) radical anion...

Although 1,2,4,5‐tetrazines or s‐tetrazines have been known in the literature for more than a century, their coordination chemistry has become increasingly popular in recent years due to their unique redox activity, multiple binding sites and their various applications. The electron‐poor character of the ring and stabilization of the radical anion through all four nitrogen atoms in their metal complexes provide new aspects in molecular magnetism towards the synthesis of new high performing Single Molecule Magnets (SMMs). The scope of this review is to examine the role of s‐tetrazine radical ligands in transition metal and lanthanide based SMMs and provide a critical overview of the progress thus far in this field. As well, general synthetic routes and new insights for the preparation of s‐tetrazines are discussed, along with their redox activity and applications in various fields. Concluding remarks along with the limitations and perspectives of these ligands are discussed.