“…Organic-based magnets were first realized through the synthesis and study of [bis(pentamethylcyclopentadienyl)iron(III)] + [tetracyanoethenide] − , [Fe III Cp 2 *] •+ [TCNE] •– , 1 , which magnetically orders below its ordering or critical temperature, T c , of 4.8 K. − Ordering as a ferromagnet was ascertained from the saturation magnetization and magnetic structure elucidated from neutron diffraction studies . The discovery of ferromagnetic ordering in an organic-based magnet (OBM) has been of significant importance to theoretical solid-state physics and shows potential for accessing multifunctional materials. − [FeCp 2 *] •+ [TCNE] −• is an electron transfer salt possessing parallel linear chains of alternating S = 1/2[FeCp 2 *] •+ cations and S = 1/2[TCNE] •– anions, with and without solvent. , Several [M III Cp 2 *] + [A] •– analogs have been synthesized through the variation of the paramagnetic metal center (M = Fe, Mn, Cr) and/or the cyanocarbon electron acceptor [A = TCNE, 7,7,8,8-tetracyano- p -quinodimethane (TCNQ), hexacyanobutadiene (HCBD), 2,3-dichloro-5,6-dicyanobenzoquinone (DDQ), and 2,3-dicyano-1,4-naphthoquinonide (DCNQ)] .…”