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JOURNAL ARTICLE
RESEARCH SUPPORT, NON-U.S. GOV'T
Understanding the Magnetic Anisotropy toward Single-Ion Magnets.
Accounts of Chemical Research 2016 November 16
Single-molecule magnets (SMMs) can retain their magnetization status preferentially after removal of the magnetic field below a certain temperature. The unique property, magnetic bistable status, enables the molecule-scale SMM to become the next-generation high-density information storage medium. SMMs' new applications are also involved in high-speed quantum computation and molecular spintronics. The development of coordination chemistry, especially in transition metal (3d) and lanthanide (4f) complexes, diversifies SMMs by introducing new ones. In both 3d and 4f SMMs, the ligands play a fundamental role in determining the SMMs' magnetic properties. The strategies for rationally designing and synthesizing high-performance SMMs require a comprehensive understanding of the effects of a crystal field. In this Account, we focus mainly on the magneto-structural correlations of 4f or 3d single-ion magnets (SIMs), within which there is only one spin carrier. These one-spin carrier complexes benefit from getting rid of exchange interactions and relatively large distances of magnetic centers in the lattice, providing the ease to construct high-performance SIMs from the crystal field perspective. We will briefly introduce the crystal field approach for 4f or 3d complexes and then the magnetic anisotropy analysis via the displaced-charge electrostatic model. This idea has been proposed for years, and the related work is also highlighted. The angular-resolved magnetometry method, predominating in determining the magnetic anisotropic axes direction, is discussed. We also give a brief introduction of the quantum chemistry ab initio method, which has shown to be powerful in understanding the magnetic anisotropy and low-lying states. In the constructing and characterizing part, we give an overview of the SIMs based on lanthanide and transition ions, reported by our group in the past 5 years. In the 4f-SIMs survey, we discuss how β-diketonates and cyclomultienes, and their combination, as ligands to influence magnetic anisotropy and provide some suggestion on designing SIMs based on different lanthanide ions. In the 3d-SIMs survey, we fully discuss the correlation between zero-field-splitting parameter D and molecular geometrical angle parameters. Finally, we lay out the challenges and further development of SIMs. We hope the understanding we provide about single-ion magnetic properties will be helpful to design high-performance SMMs.
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