Theoretical and Experimental Studies of the Magnetostructural Correlations in Mononuclear DyIII Compounds Evidenced by Quantum Tunneling of Magnetization Time, Crystal Field Parameters, and Point Charge Electrostatic Model

文献类型： 外文期刊

第一作者： Zhang, Sheng

作者： Zhang, Sheng;Tang, Jiamin;Li, Linzhou;Yao, Linbin;Zhang, Ronghu;Zhang, Ronghu;Yin, Bing

作者机构：

期刊名称：CRYSTAL GROWTH & DESIGN （ 影响因子：4.01； 五年影响因子：4.101 ）

ISSN： 1528-7483

年卷期： 2022 年 22 卷 9 期

页码：

收录情况： SCI

摘要： Three new mononuclear Dy(III) compounds with a Schiff base ligand (H2L = N,N'-bis(2-hydroxy-5-methyl-3-formylbenzyl)-N,N'-bis-(pyridin-2-ylmethyl)ethylenediamine) and different beta-diketonate co-ligands have been synthesized: [Dy(L)(tffb)] (1, tffb = 4,4,4-trifluoro-1-(2-furyl)-1,3-butanedione), [Dy(L)(fbta)] (2, fbta = 3-(4-fluorobenzoyl)-1,1,1-trifluor-oacetone), and [Dy(L)(tta)] (3, tta = thenoyltrifluoroacetone). Compounds 1-3 exhibit distorted N4O4 trigonal dodecahedron configurations with different coordination substituents leading to various axial Dy-O bond lengths and O-Dy-O bond angles. The magnetization dynamics of compounds 1-3 are apparently different. Compound 1, showing the best single-molecule magnet (SMM) properties here, has the longest tau QTM (0.357 x 10(-2) s in theory vs 0.134 x 10-2 s in experiment) and an experimentally fitted U(eff )of 94.76 K under a zero dc field. In 2 and 3, no reasonable U-eff could be fitted from the experimental data as no exponential dependence of tau on temperature is observed. This implies that the contribution of the Orbach pathway of 2 and 3 is even weaker than that of the Raman pathway. Both the accurate ab initio extraction and point charge electrostatic model show that 1 has the largest value of diagonal crystal field parameters, B20. This work verifies that the electronic structure of 1 is more suitable for SMM than 2 and 3.

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