Journal
CHEMICAL SCIENCE
Volume 7, Issue 1, Pages 684-691Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5sc02986d
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Funding
- NSFC [21290171, 21321001, 21102039, 21571008, 21572048]
- National Basic Research Program of China [2013CB933401, 2010CB934601]
- BNLMS [20140108]
- Educational Commission of Heilongjiang Province [1254G045, 12541639]
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A series of mononuclear lanthanide Zn-Dy-Zn type single-molecule magnets (SMMs) were synthesized and magnetically characterized. The four molecules ([Zn-2(L-1)(2)DyCl3]center dot 2H(2)O (1), [Zn-2(L-1)(2)Dy(MeOH)Br-3]center dot 3H(2)O (2), [Zn-2(L-1)(2)Dy(H2O)Br-2]center dot[ZnBr4](0.5) (3) and [Zn-2(L-2)(2)DyCl3]center dot 2H(2)O (4)) all display remarkable magnetic relaxation behavior with a relatively high energy barrier and hysteresis temperature, despite possessing a low local geometry symmetry of the center Dy(III) ions. Ab initio studies revealed that the symmetry of the charge distribution around the Dy(III) ion is the key factor to determine the relaxation of the SMMs. The four complexes orient their magnetic easy axes along the negative charge-dense direction of the first coordination sphere. The entire molecular magnetic anisotropy was therefore controlled by a single substituent atom in the hard plane which consists of five coordination atoms (perpendicular to the easy axis), and the lower charge distribution on this hard plane in combination with the nearly coplanarity of the five coordination atoms ultimately lead to the prominent magnetic slow relaxation. This offers an efficient and rational method to improve the dynamic magnetic relaxation of the mononuclear lanthanide SMMs that usually possess a low local geometry symmetry around the lanthanide(III) center.
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