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These triplesalen ligands provide three salen\u2010like coordination environments bridged in a <jats:italic>meta<\/jats:italic>\u2010phenylene arrangement by a phloroglucinol backbone. The structure of [(talen)Cu<jats:sup>II<\/jats:sup><jats:sub>3<\/jats:sub>] (<jats:bold>1<\/jats:bold>) was communicated recently. The structure of the <jats:italic>tert<\/jats:italic>\u2010butyl derivative [(talen<jats:inline-graphic xmlns:xlink=\"http:\/\/www.w3.org\/1999\/xlink\" xlink:href=\"graphic\/tex2gif-sup-10.gif\" xlink:title=\"urn:x-wiley:09476539:media:CHEM200700781:tex2gif-sup-10\"\/>)Cu<jats:sup>II<\/jats:sup><jats:sub>3<\/jats:sub>] (<jats:bold>2<\/jats:bold>) was established in three different solvates. The molecular structures of these trinuclear complexes show notable differences, the most important of which is the degree of ligand folding around the central Cu<jats:sup>II<\/jats:sup>\u2013phenolate bonds. This folding is symmetric with regard to the central phloroglucinol backbone in two structures, where it gives rise to bowl\u2010shaped overall geometries. For one solvate two trinuclear triplesalen complexes form a supramolecular disk\u2010like arrangement, hosting two dichloromethane molecules like two pearls in an oyster. The FTIR spectra of these complexes indicate the higher effective nuclear charge of Cu<jats:sup>II<\/jats:sup> in comparison to the trinuclear Ni<jats:sup>II<\/jats:sup> complexes by the lower C\uf8ffO and higher C\uf8feN stretching frequencies. The UV\/Vis\/NIR spectra of <jats:bold>1<\/jats:bold>\u2013<jats:bold>3<\/jats:bold> reflect the stronger ligand folding in the <jats:italic>tert<\/jats:italic>\u2010butyl complex <jats:bold>2<\/jats:bold> by an intense phenolate\u2010to\u2010Cu<jats:sup>II<\/jats:sup> LMCT. This absorption is absent in <jats:bold>1<\/jats:bold> and is obscured by the nitro chromophore in <jats:bold>3<\/jats:bold>. The more planar molecular structures cause orthogonality of the Cu<jats:sup>II<\/jats:sup> d<jats:inline-graphic xmlns:xlink=\"http:\/\/www.w3.org\/1999\/xlink\" xlink:href=\"graphic\/tex2gif-inf-14.gif\" xlink:title=\"urn:x-wiley:09476539:media:CHEM200700781:tex2gif-inf-14\"\/> orbital and the phenolate O p<jats:sub><jats:italic>z<\/jats:italic><\/jats:sub> orbital, which leads to small LMCT dipole strengths. Whereas <jats:bold>1<\/jats:bold> and <jats:bold>3<\/jats:bold> exhibit only irreversible oxidations, <jats:bold>2<\/jats:bold> exhibits a reversible one\u2010electron oxidation at +0.26\u2005V, a reversible two\u2010electron oxidation at +0.59\u2005V, and a reversible one\u2010electron oxidation at +0.81\u2005V versus Fc<jats:sup>+<\/jats:sup>\/Fc. The one\u2010electron oxidized form <jats:bold>2<\/jats:bold><jats:sup>+<\/jats:sup> is strongly stabilized with respect to reference mononuclear salen\u2010like Cu complexes. Chemical one\u2010electron oxidation of <jats:bold>2<\/jats:bold> to <jats:bold>2<\/jats:bold><jats:sup>+<\/jats:sup> allows the determination of its UV\/Vis\/NIR spectrum, which indicates a ligand\u2010centered oxidation that can be assigned to the central phloroglucinol unit by analogy with the trinuclear Ni triplesalen series. Delocalization of this oxidation over three Cu<jats:sup>II<\/jats:sup>\u2013phenolate subunits causes the observed energetic stabilization of <jats:bold>2<\/jats:bold><jats:sup>+<\/jats:sup>. Temperature\u2010dependent magnetic susceptibility measurements reveal ferromagnetic couplings for all three trinuclear Cu<jats:sup>II<\/jats:sup> triplesalen complexes. The trend of the coupling constants can be rationalized by two opposing effects: 1)\u2005electron\u2010withdrawing terminal substituents stabilize the central Cu<jats:sup>II<\/jats:sup>\u2013phenolate bond, which results in a stronger coupling, and 2)\u2005ligand folding around the central Cu<jats:sup>II<\/jats:sup>\u2013phenolate bond opens a bonding pathway between the magnetic Cu<jats:sup>II<\/jats:sup> d<jats:inline-graphic xmlns:xlink=\"http:\/\/www.w3.org\/1999\/xlink\" xlink:href=\"graphic\/tex2gif-inf-16.gif\" xlink:title=\"urn:x-wiley:09476539:media:CHEM200700781:tex2gif-inf-16\"\/> orbital and the phenolate O p<jats:sub><jats:italic>z<\/jats:italic><\/jats:sub> orbital, which results in a stronger coupling. Density functional calculations indicate that both spin\u2010polarization and spin\u2010delocalization are operative and that slight geometric variations alter their relative magnitudes.<\/jats:p>","DOI":"10.1002\/chem.200700781","type":"journal-article","created":{"date-parts":[[2007,10,15]],"date-time":"2007-10-15T11:53:54Z","timestamp":1192449234000},"page":"9191-9206","source":"Crossref","is-referenced-by-count":85,"title":["Trinuclear Copper Complexes with Triplesalen Ligands: Geometric and Electronic Effects on Ferromagnetic Coupling via the Spin\u2010Polarization 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