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Fine-Tuning of the Coordination Environment To Regulate the Magnetic Behavior in Solvent/Anion-Dependent DyIII
Lin Sun1, Sheng Zhang1,2, Chengfang Qiao1,3
1Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education, College of Chemistry and Materials Science, Northwest University , Xi'an, Shaanxi 710127, China.
Abstract:
It is crucial to understand and elucidate the self-assembly mechanism in solution systems for the construction of DyIII-based single-molecule magnets (SMMs). Herein, through fine-tuning of the anion and solvent, we prepared three nine-coordinate mononuclear dysprosium compounds, [Dy(2,3'-pcad)(NO3)2(CH3OH)2] (1), [Dy(2,3'-Hpcad)2(H2O)3]·3Cl·5H2O (2), and [Dy(2,3'-pcad)(NO3)(H2O)4]·NO3·H2O (3) [2,3'-Hpcad = N3-(2-pyridoyl)-3-pyridinecarboxamidrazone]. The reactions of formation for 1-3 are in situ thermodynamically monitored by isothermal titration calorimetry. Magnetic data analysis reveals that 2 shows SMM behavior under a zero direct-current (dc) field, whereas 1 and 3 exhibit distinct slow magnetic relaxation processes upon a 1200 Oe dc field. To deeply understand the different magnetic behaviors, the magnetic anisotropy of 1-3 has been systematically studied by ab initio calculations, which is consistent with the experimental observations. Moreover, the semiconductor behaviors of 1-3 have been investigated by experimental measurements of UV-vis spectroscopy.
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