Journal
INORGANIC CHEMISTRY
Volume 61, Issue 25, Pages 9785-9791Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.2c01299
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Funding
- National Key R&D Program of China [2018YFA0306002]
- National Natural Science Foundation of China [21971123, 21973046]
- Natural Science Foundation of Tianjin [18JCJQJC47200]
- Ministry of Education of China [B12015]
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Two mononuclear D-III single-molecule magnets with different ligand substituents exhibit similar coordination environments but different magnetization dynamics. The energy gap of 2 is higher than 1, leading to a lower relaxation rate of magnetization through quantum tunneling.
Two mononuclear D-III single-molecule magnets with different ligand substituents located far from the coordinating atoms, [Dy(L-NO2)(NO3)] (1) and [Dy(L-Me)(NO3)] (2), and their diamagnetic-ion diluted analogues, 1' and 2', were structurally and magnetically characterized. 1 and 2 have nearly identical coordination environments of D-III ions with D-2d symmetry but different magnetization dynamics. No Orbach process was observed for 1 and 1' in the testing temperature and frequency range, but effective energy barriers of 575 and 829 K for 2 and 2' were obtained, respectively. The opened hysteresis loops were observed until 6 K for 1 and 10 K for 2. Ab initio calculations reveal that the energy gaps between ground and low-lying excited states of 2 are higher than those of 1 and the relaxation rate through quantum tunneling of magnetization of 2 is lower than that of 1 due to the electronic effect of the axial coordinating oxygen atoms influenced by ligand substitutions.
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