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• W2068710701 abstract "The reaction of the tris(tetradentate) triplesalen ligand H6talent-Bu2, which provides three salen-like coordination environments bridged in a meta-phenylene arrangement by a phloroglucinol backbone, with MnII salts under aerobic conditions, affords, in situ, the trinuclear MnIII triplesalen complex [(talent-Bu2){MnIII(solv)n}3]3+. This species then reacts with [(Me3tacn)Cr(CN)3] to form the tetranuclear complex [{(talent-Bu2)MnIII3}{(Me3tacn)Cr(CN)3}]3+ ([MnIII3CrIII]3+). The regular ligand folding observed in the trinuclear triplesalen complex preorganizes the three metal ions for the reaction with three facially coordinated nitrogen atoms of [(Me3tacn)Cr(CN)3]. [{(talent-Bu2)(MnIII(MeOH))3}{(Me3tacn)Cr(CN)3}](ClO4)3 (1) was characterized by infrared spectroscopy, elemental analysis, mass spectrometry, electron absorption spectroscopy, and magnetic measurements. The molecular structure was established for the acetate-substituted derivative [{(talent-Bu2)(MnIII(MeOH))2(MnIII(OAc))}{(Me3tacn)Cr(CN)3}](ClO4)2 (2) by single-crystal X-ray diffraction. Variable-temperature−variable-field and μeff versus T magnetic data have been analyzed in detail by full-matrix diagonalization of the appropriate spin-Hamiltonian, consisting of isotropic exchange, zero-field splitting, and Zeeman interaction components. Satisfactory reproduction of the experimental data has been obtained for the parameters JMn−Cr = −0.12 ± 0.04 cm−1, JMn−Mn = −0.70 ± 0.03 cm−1, and DMn = −3.0 ± 0.4 cm−1. These generate a triply degenerate pseudo St = 7/2 spin manifold, which cannot be appropriately described by a giant spin model and which exhibits a weak easy-axis magnetic anisotropy. This is corroborated by the onset of a frequency-dependent χ′′ signal at low temperatures, demonstrating a slow relaxation of the magnetization indicative of 1 being a single-molecule magnet. Comparing the properties to those of the heptanuclear analogue [{(talent-Bu2)MnIII3}2{CrIII(CN)6}]3+ ([MnIII6CrIII]3+) formed by the reaction of 2 equiv of [(talent-Bu2){MnIII(solv)n}3]3+ with 1 equiv of [Cr(CN)6]3− [Glaser, T.; Heidemeier, M.; Weyhermüller, T.; Hoffmann, R.-D.; Rupp, H.; Müller, P. Angew. Chem. Int. Ed., 2006, 45, 6033−6037] demonstrates a lower driving force for formation, a strongly reduced JMn−Cr exchange, a slightly reduced JMn−Mn exchange, and a significantly longer Mn−NN≡C bond length in [MnIII3CrIII]3+. Taking into account magneto-structural correlations establishes a supramolecular interaction between the two [(talent-Bu2)MnIII3]3+ subunits in [MnIII6CrIII]3+ responsible for the structural distortion and the short Mn−NN≡C distance which results in a strong JMn−Cr exchange and thus [MnIII6CrIII]3+ being a single-molecule magnet with a relatively high effective anisotropy barrier of 25.4 K." @default.
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• W2068710701 date "2009-10-05" @default.
• W2068710701 modified "2023-10-18" @default.
• W2068710701 title "Synthesis, Structure, and Magnetic Characterization of a <i>C</i>₃-Symmetric Mn^III₃Cr^III Assembly: Molecular Recognition Between a Trinuclear Mn^III Triplesalen Complex and a <i>fac</i>-Triscyano Cr^III Complex" @default.
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• W2068710701 doi "https://doi.org/10.1021/ic901148q" @default.
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