期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 23, 期 70, 页码 17775-17787出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201703755
关键词
dysprosium; magnetic relaxation; Schiff base ligands; single-ion magnets; superparamagnetic behavior
资金
- National Natural Science Foundation of China [21727805, 21673180, 21373162, 21673181, 21473135, 21103137]
Taking advantage of the steric hindrance and charge-driving effects, four air-stable pentagonal bipyramidal mononuclear Dy-III compounds were hydrothermally synthesized. With a tetradentate ligand, N,N'-bis(2-methylenepyridinyl)ethylenediamine (Bpen), invariably coordinates to Dy-III in an equatorial plan, 1-3 achieve an orderly transformation of the ligand field by sequentially replacing the remaining sites of the Dy-III ion. Compound 4 possesses the same coordination atoms but a different peripheral coordination sphere with 3. Magnetic characterizations display that the compounds are field-induced single-ion magnets (SIM) with actually low barriers, even though 2 has both the same atoms and a similar geometry of the first sphere compared with [Dy(bbpen)Cl] (2, H(2)bbpen=N,N'-bis(2-hydroxybenzyl)-N,N'-bis(2-methylpyridyl)ethylenediamin), a high-performance SIM previously reported. Detailed ab initio calculations have been employed to further elucidate the electronic and magnetic structure of the low-lying energy levels of compounds 1-4 and 2'. The theoretical results indicate there is an apparent difference in the electronic structure for these compounds. The analysis on the electrostatic potential further demonstrates that although the pentagonal bipyramidal D-5h is one of the ideal configurations expected, the electron density of the donor atoms from the different hybridizations and other functional groups, outside the first sphere, should also be considered in the rational design of promising molecular magnets.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据