4.6 Article

Trinuclear Cyanido-Bridged [Cr2Fe] Complexes: To Be or not to Be a Single-Molecule Magnet, a Matter of Straightness

Journal

CHEMISTRY-A EUROPEAN JOURNAL
Volume 27, Issue 62, Pages 15484-15495

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202102571

Keywords

ab initio calculations; anisotropy; magnetism; pentagonal bipyramid; single-molecule magnets

Funding

  1. French National Research Agency, ANR [ANR-17-CE07-0007]

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Trinuclear metal complexes were synthesized to investigate their influence on the magnetic anisotropy of Fe-II derivatives and their Single-Molecule Magnet behaviors, revealing a significant effect of the bending of M-N to C linkages on the slow relaxation of magnetization in [Cr2Fe] complexes. Theoretical calculations emphasized the importance of apical C-N-Fe linkages on the magnetic anisotropy and exchange interactions in these complexes.
Trinuclear systems of formula [{Cr(L-N3O2Ph)(CN)(2)}(2)M(H2LN3O2R)] (M=Mn-II and Fe-II, L-N3O2R stands for pentadentate ligands) were prepared in order to assess the influence of the bending of the apical M-N equivalent to C linkages on the magnetic anisotropy of the Fe-II derivatives and in turn on their Single-Molecule Magnet (SMM) behaviors. The cyanido-bridged [Cr2M] derivatives were obtained by assembling trans-dicyanido Cr-III complex [Cr(L-N3O2Ph)(CN)(2)](-) and divalent pentagonal bipyramid complexes [M-II(H2LN3O2R)](2+) with various R substituents (R=NH2, cyclohexyl, S,S-mandelic) imparting different steric demand to the central moiety of the complexes. A comparative examination of the structural and magnetic properties showed an obvious effect of the deviation from straightness of the M-N equivalent to C alignment on the slow relaxation of the magnetization exhibited by the [Cr2Fe] complexes. Theoretical calculations have highlighted important effects of the bending of the apical C-N-Fe linkages on both the magnetic anisotropy of the Fe-II center and the exchange interactions with the Cr-III units.

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