Alignment of Axial Anisotropy in a 1D Coordination Polymer shows Improved Field Induced Single Molecule Magnet Behavior over a Mononuclear Seven Coordinated Fe Complex.

Herein, we report a CN-bridged alternating Fe -Ni 1D chain to ensure the alignment of axial anisotropy and improve the single molecule magnet (SMM) behavior in seven coordinated Fe compound. The chain was constructed from hepta coordinated Fe(II) complex as an anisotropic building unit and diamagnetic nickel tetra cyanate as a bridging ligand. The magnetic measurements show the easy-axis anisotropy of the seven coordinated Fe(II) complex and field induced SMM behavior with spin reversal energy barrier U =61(2) K (42 cm ) and pre-exponential relaxation time τ =1.9×10  s. The detailed analysis of the relaxation dynamics discloses that the Orbach process plays an important role in slow relaxation of magnetization for this compound. Notably, this example represents a remarkable energy barrier observed in hepta coordinated Fe(II) SMMs. The ab initio calculations estimate the magnitude of axial anisotropy and show the parallel orientation of the anisotropic axis throughout the 1D polymeric chain. In addition, it is also reported that the presence of weak π accepter ligands in the distorted axial position enhance the easy-axis anisotropy.