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Rational design of a photomagnetic chain: Bridging single-molecule magnets with a spin-crossover complex

AutorPichon, Céline; Roubeau, Olivier; Mathonière, Corine; Clérac, Rodolphe
Fecha de publicación2013
EditorAmerican Chemical Society
CitaciónJournal of the American Chemical Society 135(39): 14840-14853 (2013)
ResumenThe spin-crossover complex [Fe(LN5)(CN)2] ·H2O (1, LN5 = 2,13-dimethyl-3,6,9-12,18- pentaazabicyclo[12.3.1]octadeca-1(18),2,12,14,16-pentaene), reported previously by Nelson et al. in 1986, was reinvestigated, and its structure determined by single crystal X-ray diffraction for the first time. The reaction between [MnIII(saltmen)(H2O)]+ and this photomagnetic linker yielded the trinuclear molecular complex [{Mn(saltmen)} 2FeHS(LN5)(CN)2](ClO 4)2·0.5CH3OH (2) and the one-dimensional compound [{Mn(saltmen)}2FeLS(LN5)(CN) 2](ClO4)2·0.5C4H 10O·0.5H2O (3) depending on the addition order of the reagents (HS: High-Spin; LS: Low-Spin). Compound 3 exhibits a wave-shaped chain structure built from the assembly of the trinuclear [Mn III-NC-FeII] motif found in 2. Static magnetic measurements revealed the existence of antiferromagnetic Mn III···FeII (FeII HS, S = 2) interactions in the trinuclear entity of 2 via the cyanido bridge leading to an ST = 2 ground state. In the case of 3, concomitant ferromagnetic and antiferromagnetic exchange interactions are found along the chain due to the presence of two crystallographically independent {Mn2(saltmen) 2} units, which behave differently as shown by the magnetic susceptibility analysis, while the FeII (LS, S = 0) cyanido-bridging moiety is isolating these dinuclear MnIII units. ac susceptibility experiments indicated slow relaxation of the magnetization arising from the ferromagnetically coupled [Mn2] units (τ0 = 1.1 × 10-7 s and Δeff/kB = 13.9 K). Optical reflectivity and photomagnetic properties of 1 and 3 have been investigated in detail. These studies reveal that the photomagnetic properties of 1 are kept after its coordination to the acceptor MnIII/saltmen complexes, allowing in 3 to switch >on> and >off> the magnetic interaction between the photoinduced FeII HS unit (S = 2) and the Mn(III) ions. To the best of our knowledge, the compound 3 represents the first example of a coordination network of single-molecule magnets linked by spin-crossover units inducing thermally and photoreversible magnetic and optical properties. © 2013 American Chemical Society.
Descripciónet al.
Identificadoresdoi: 10.1021/ja407570n
issn: 0002-7863
e-issn: 1520-5126
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