First magnets based on thiocyanato-bridges.

2-D NCS-bridged {3d-4d} molecule-based magnets, formed by reaction of [Mo(III)(NCS)(6)](3-) with either Ni(II) or Co(II) complexes, have been found to exhibit magnetic ordering with T(C) = 39 K for {Co(3)Mo(2)} while {Ni(3)Mo(2)} has a non-magnetic ground state as a result of exact compensation by the individual sub-lattices.

Substantial exchange coupling for {Mo-NCS-M} combination: illustration for 1-D [{Mo(NCS)6}{NiL}2(NCS)]n.

An antiferromagnetic interaction of J = -51 cm(-1) has been obtained in a NCS-bridged {Mo(III)-Ni} compound (i.e. [{Mo(NCS)(6)}{NiL}(2)(NCS)](n)), a value twice as large as for the homologous {Cr(III)-Ni} derivative.