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MnII(TCNE)3/2(I3)1/2 and MnII(TCNE)[C4(CN)8]1/2 [tetracyanoethylene (TCNE)] are organic‐based magnets with 3D and 2D extended network structures with vastly different magnetic behavior. They have similar ferrimagnetic coupled layers of MnII(TCNE)•− with different interlayer couplings, which lead, respectively, to net ferrimagnetic (Tc = 171 K) and antiferromagnetic (Tc = 68 K) order.
Joel Miller, Peter Stephens, and co‐workers report on p. 2514 on MnII(TCNE)3/2I3/2(TCNE = tetracyanoethylene), which is a ferrimagnet at a surprisingly high temperature of 0 °C under pressure. It has a 3D network structure with each Mn ion coordinated to six TCNE radicals, leading to strong spin coupling and ferrimagnetic behavior. This composition/structure is the Rosetta stone for understanding...
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