Investigating the Unconventional Ferrimagnetic Ordering in the Molecular-based Magnet, V(TCNE)₂

The insulating ferrimagnet, vanadium tetracyanoethylene (V(TCNE)₂) has been used to demonstrate on-chip integration of ultra-low loss magnons into superconducting quantum devices and circuits, opening the door to the exploitation of time-reversal symmetry breaking and other magnetic functionality in emerging quantum technologies [1]. Further, recent studies have advanced our understanding of its electronic structure and consequent impact on static and dynamic magnetic properties [2]. These findings point to the combination of strong magnetic order (ordering temperature above 600 K) and extremely low spin density (saturation magnetization of 110 G) due to its porous structure, as key drivers of this functionality and indicate V(TCNE)₂ is a representative of an underexplored class of metal-organic framework (MOF) magnets [3]. Here, we present further experimental investigation of the magnetic order in V(TCNE)₂ as a function of growth condition that provides additional insight into the mechanisms governing the metal-ligand antiferromagnetic exchange and low-loss magnon excitations in this unique regime of magnetic materials.