Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 27, Pages 10077-10082Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c05279
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Funding
- Key Research Program of Frontier Sciences, CAS [ZDBS-LY-SLH023]
- National Natural Science Foundation of China [21525103, 21871247, 21973046, 11774178]
- Royal Society-Newton Advanced Fellowship [NA160075]
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By introducing fluorinated substituents on the ligands, two chiral Dy(III) macrocyclic complexes with high anisotropy barrier and relaxation time were obtained, providing a new avenue for improving air-stable SMMs and depositing SMMs on surfaces.
Design and synthesis of air-stable and easily tailored high-performance single-molecule magnets (SMMs) are of great significance toward the implementation of SMMs in molecular-based magneto-electronic devices. Here, by introducing electron-withdrawing fluorinated substituents on equatorial ligand, two chiral Dy(III) macrocyclic complexes, RRRR-Dy-D6hF12 (1) and SSSS-Dy-D6hF12 (2), with a record anisotropy barrier exceeding 1800 K and the longest relaxation time approaching 2500 s at 2.0 K for all known air-stable SMMs, were obtained. The nearly perfect axiality of the ground Kramers doublet (KD) enables the open hysteresis loops up to 20 K in the magnetically diluted sample. It is notable that they are structurally rigid with high thermal stability and the apical ligand can be tailored to carry proper surface-binding groups. This finding not only improves the magnetic properties for air-stable SMMs but also provides a new avenue for deposition of SMMs on surfaces.
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