Inducing Ferrimagnetic Exchange in 1D-FeSe 2 Chains Using Heteroleptic Amine Complexes: [Fe(en)(tren)][FeSe 2 ] 2 .

[Fe(en)(tren)][FeSe 2 ] 2 ( en = ethylenediamine, C 2 H 8 N 2 , tren = tris(2-aminoethyl)amine, C 6 H 18 N 4 ) has been synthesized by a mixed-ligand solvothermal method. Its crystal structure contains heteroleptic [Fe(en)(tren)] 2+ complexes with distorted octahedral coordination, incorporated between 1D-FeSe 2 chains composed of edge-sharing FeSe 4 tetrahedra. The twisted octahedral coordination environment of the Fe-amine complex leads to partial dimerization of Fe-Fe distances in the FeSe 2 chains so that the FeSe 4 polyhedra deviate strongly from the regular tetrahedral geometry. 57 Fe Mössbauer spectroscopy reveals oxidation states of +3 for the Fe chain atoms and +2 for the Fe complex atoms. The close proximity of Fe atoms in the chains promotes ferromagnetic nearest neighbor interactions, as indicated by a positive Weiss constant, θ = +53.8(6) K, derived from the Curie-Weiss fitting. Magnetometry and heat capacity reveal two consecutive magnetic transitions below 10 K. DFT calculations suggest that the ordering observed at 4 K is due to antiferromagnetic intra chain interactions in the 1D-FeSe 2 chains. The combination of two different ligands creates an asymmetric coordination environment that induces changes in the structure of the Fe-Se fragments. This synthetic strategy opens new ways to explore the effects of ligand field strength on the structure of both Fe- amine complexes and surrounding Fe-Se chains.