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Interchange between coordinated and lattice solvents generates the highest energy barrier within nine-coordinated DyIII single molecule magnets

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Abstract

It is crucial to promote axiality to enhance easy-axis magnetic anisotropy. Two mononuclear DyIII compounds, in which each DyIII is nine-coordinated, namely, [(C12H10N5O)Dy(NO3)2(H2O)2]·C2H5OH (1) and [(C12H10N5O)Dy(NO3)2(C2H5OH)2]·H2O (2) (HL = N3-(2-pyridoyl)-4-pyridinecarboxamidrazone), have been prepared through controlling the amount of C2H5OH and H2O solvents. Geometry modulations were realized by interchanging coordinated and lattice solvents, thus achieving a structure closer to the configuration of a capped square antiprism for 2 compared to that for 1. Notably, magnetic studies revealed that compound 1 displays no slow relaxation of magnetization while compound 2 exhibits single-molecule magnet (SMM) behaviour in the absence of a static magnetic field, with the highest energy barrier (203.11 K) of nine-coordinated DyIII SMMs. Ab initio calculations were performed to elucidate such a distinct performance, demonstrating that the combination of the larger charge distribution along the magnetic axis and the lower charge distribution in the equatorial plane generates a strong easy-axis ligand field to enhance magnetic properties, which is further associated with the structural symmetry. In addition, a possible coordination mode is proposed to realize high axis anisotropy for nine-coordinated DyIII compounds. This work presents an effective method to modulate the dynamic magnetic relaxation of the DyIII SMMs through interchange between coordinated and lattice solvents.

Graphical abstract: Interchange between coordinated and lattice solvents generates the highest energy barrier within nine-coordinated DyIII single molecule magnets

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Publication details

The article was received on 01 Jul 2017, accepted on 01 Aug 2017 and first published on 02 Aug 2017


Article type: Communication
DOI: 10.1039/C7DT02382K
Citation: Dalton Trans., 2017, Advance Article
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    Interchange between coordinated and lattice solvents generates the highest energy barrier within nine-coordinated DyIII single molecule magnets

    L. Sun, S. Zhang, Z. Jiang, Q. Yang, S. Chen, Y. Zhang, W. Wang, Q. Wei and G. Xie, Dalton Trans., 2017, Advance Article , DOI: 10.1039/C7DT02382K

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