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Electrostatic bending and outer-sphere intervalence transfer in a flexible ligand-bridged ruthenium(III)-iron(II) complex

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In the mixed-valence complex [RuIII(NH3)5(μ-dpypn)FeII(CN)5] with the flexible bridging ligand 1,3-di(4-pyridyl)propane (dpypn), electrostatic interactions between the {Ru(NH3)5}3+ and {Fe(CN)5}3− moieties drive a strong bending of dpypn and approximation of the RuIII and FeII centers, from which the enhanced electronic coupling between metal ions produces an intense intervalence-transfer absorption in the near-infrared region. Density functional theory calculations corroborate both the electrostatic bending in this heterobinuclear complex and a linear geometry in the homobinuclear counterparts [Ru(NH3)5(μ-dpypn)Ru(NH3)5]5+ and [Fe(CN)5(μ-dpypn)Fe(CN)5]5−, for which no evidence of electronic coupling was found because of the separation between metal centers. Furthermore, the heterobinuclear species formed an inclusion complex with β-cyclodextrin where the imposed linear geometry prevents significant electronic coupling and intervalence charge transfer between the RuIII and FeII centers.
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Keywords: Outer-sphere intervalence transfer; electrostatic configurational bending; mixed valency; pentaammineruthenium complexes; pentacyanidoferrate complexes

Document Type: Research Article

Affiliations: 1: Instituto de Química, Universidade de São Paulo, São Paulo, Brazil; 2: Los Alamos National Laboratory, Los Alamos, NM, USA

Publication date: July 3, 2018

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