Journal
ADVANCED SCIENCE
Volume 6, Issue 20, Pages -Publisher
WILEY
DOI: 10.1002/advs.201901352
Keywords
antiferromagnetic; dysprosium; exchange interactions; metallofullerene; oxide; single molecule magnets
Categories
Funding
- National Science Foundation China [NSFC51302178]
- NSF of Jiangsu Province [BK20171211]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (grant PAPD)
- project of scientific and technologic infrastructure of Suzhou [SZS201708]
- European Union, European Research Council [648295]
- Marie Skodowska-Curie action [748635]
- Deutsche Forschungsgemeinschaft [PO 1602/4-1, PO 1602/5-1]
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A new class of single-molecule magnets (SMMs) based on Dy-oxide clusterfullerenes is synthesized. Three isomers of Dy2O@C-82 with C-s(6), C-3v(8), and C-2v(9) cage symmetries are characterized by single-crystal X-ray diffraction, which shows that the endohedral Dy-(mu(2)-O)-Dy cluster has bent shape with very short Dy-O bonds. Dy2O@C-82 isomers show SMM behavior with broad magnetic hysteresis, but the temperature and magnetization relaxation depend strongly on the fullerene cage. The short Dy-O distances and the large negative charge of the oxide ion in Dy2O@C-82 result in the very strong magnetic anisotropy of Dy ions. Their magnetic moments are aligned along the Dy-O bonds and are antiferromagnetically (AFM) coupled. At low temperatures, relaxation of magnetization in Dy2O@C-82 proceeds via the ferromagnetically (FM)-coupled excited state, giving Arrhenius behavior with the effective barriers equal to the AFM-FM energy difference. The AFM-FM energy differences of 5.4-12.9 cm(-1) in Dy2O@C-82 are considerably larger than in SMMs with {Dy2O2} bridges, and the Dy...Dy exchange coupling in Dy2O@C-82 is the strongest among all dinuclear Dy SMMs with diamagnetic bridges. Dy-oxide clusterfullerenes provide a playground for the further tuning of molecular magnetism via variation of the size and shape of the fullerene cage.
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