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Article Dans Une Revue Inorganic Chemistry Année : 2010

Electronic and Magnetic Study of Polycationic Mn-12 Single-Molecule Magnets with a Ground Spin State S=11

Résumé

The preparation, magnetic characterization, and X-ray structures of two polycationic Mn-12 single-molecule magnets (Mn12O12(bet)(16)(EtOH)(4)](PF6)(14)center dot 4CH(3)CN center dot H2O (1) and [Mn12O12(bet)(16)(EtOH)(3)(H2O)](PF6)(13)(OH)center dot 6CH(3)CN center dot EtOH center dot H2O (2) (bet = betaine = (CH3)(3)N+-CH2-CO2-) are reported. 1 crystallizes in the centrosymmetric P2/cspace group and presents a (0:2:0:2) arrangement of the EtOH molecules in its structure. 2 crystallizes in the noncentrosymmetric P (4) over bar space group with two distinct Mn-12 polycations, [Mn12O12(bet)(16)(EtOH)(2)(H2O)(2)](14+) (2A) and [Mn12O12(bet)(16)(EtOH)(4)](14+)(2B) per unit cell. 2A and 2B show a (1:1:1:1) distribution of the coordinated solvent molecules. Interestingly, bond valence sum calculations extracted from X-ray diffraction data indicate the presence of two Mn2+ ions in the Mn2+ core for both 1 and 2. This finding is confined by X-ray absorption spectroscopy (XAS) measurements. A complete magnetic characterization, including subkelvin micro-SQUID magnetometry and inelastic neutron scattering (INS) measurements, permits to extract the parameters of the giant spin Hamiltonian of these polycations. Compared with the archetypal Mn2+ acetate, an increase in the value of the ground spin state from S = 10 to S = 11 together with a decrease in the effective energy barrier, is observed for 1 and 2. Such a result is consistent with the reduction of two Mn3+ to the less anisotropic Mn2+ ion in the structures.
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Dates et versions

hal-00979712 , version 1 (16-04-2014)

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J.M. Clemente-Juan, Eugenio Coronado, Alicia Forment-Aliaga, Alejandro Gaita-Arino, Carlos Giménez-Saiz, et al.. Electronic and Magnetic Study of Polycationic Mn-12 Single-Molecule Magnets with a Ground Spin State S=11. Inorganic Chemistry, 2010, 49 (2), pp.386-396. ⟨10.1021/ic901824d⟩. ⟨hal-00979712⟩

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