Persistent Metal Bis(Hexafluoroacetylacetonato) Complexes Featuring a 2,2′-Bipyridine Substituted Triarylamminium Radical Cation AdugnaSharew RevunovaKseniya DjukicBrandon GorelskySerge I. JenkinsHilary A. LemaireMartin T. 2010 Herein, we describe the preparation of a 2,2′-bipyridine derivative containing a redox-active <i>N</i>,<i>N</i>′-(4,4′-dimethoxydiphenylamino) substituent (<b>1</b>), which readily coordinates M(hfac)<sub>2</sub> salts [M = Mn (<b>2</b>), Ni (<b>3</b>), Cu (<b>4</b>)] to generate stable, neutral, and pseudo-octahedral coordination complexes, which have been fully characterized. Cyclic voltammetry and spectroelectrochemical measurements on complexes <b>2</b>−<b>4</b> indicate stable one-electron oxidation processes, and the formation of persistent radical cation complexes. The neutral complexes (M = Mn or Ni) were subject to one-electron oxidation with NOPF<sub>6</sub> in acetonitrile, and magnetic moments of the resulting solutions were obtained using the Evans method at different temperatures. Our experimental results suggest that the first reported ferromagnetically coupled metal−triarylamminum radical cation complex is obtained when M = Mn<sup>2+</sup>, and antiferromagnetic coupling results when M = Ni<sup>2+</sup>. These results are supported by results from density functional theory calculations, which indicate that a π spin polarization mechanism for magnetic exchange coupling is operative in singly oxidized complexes, <b>2</b>−<b>4</b>.