Structural and Magnetic Characterisation of [Fe(Cp*)2][Ni(dmio)2]·THF

The crystal structure of [Fe(Cp*) 2 ][Ni(dmio) 2 ].THF consists of 2D layers composed of parallel chains, where side-by-side pairs of donors alternate with the acceptors, ..D + D + A - D + D + A - ... In these chains there is a net charge (+) per repeat unit (D + D + A - ) and these layers are separated by acceptor layers. The magnetic behaviour of [Fe(Cp*) 2 ][Ni(dmio) 2 ].THF is dominated by FM interactions, which are attributed to the DA intrachain interactions.