Journal ArticleDOI
Ligand field fine-tuning on the modulation of the magnetic properties and relaxation dynamics of dysprosium(III) single-ion magnets (SIMs): synthesis, structure, magnetism and ab initio calculations
Sheng Zhang,Sheng Zhang,Haipeng Wu,Lin Sun,Hongshan Ke,Sanping Chen,Bing Yin,Qing Wei,Desuo Yang,Shengli Gao +9 more
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TLDR
In this paper, the magnetic properties of Dy(III-SIMs were investigated by ab initio calculations and the magnetic anisotropy of 1−4 was investigated by showing that the capping ligands could play an important role in the fine tuning of the SMM property via an effect on the equatorial electrostatic potential.Abstract:
To fine-tune the magnetic anisotropy and further modulate the magnetic properties and relaxation dynamics of dysprosium(III) single-ion magnets (SIMs), it is crucial to explore their controllable synthesis and conduct a systematic theoretical investigation. Herein, the mononuclear Dy(III) precursor, [Dy(DMF)2(tffb)3] (tffb = 4,4,4-trifluoro-1-(4-fluorophenyl)-1,3-butanedione), as a “metalloligand” towards different capping ligands, affords two new mononuclear Dy(III) complexes in different solvent systems, [Dy(bpy)(tffb)3]·(C4H8O2)1/3 (1) and [Dy(Phen)(tffb)3] (2) (bpy = 2,2′-bipyridine, Phen = 1,10-phenanthroline). Using 4,4,4-trifluoro-1-(4-methylphenyl)-1,3-butanedione (tfmb) as a ligand with the coligand bpy, [Dy(bpy)(tfmb)3] (3) is obtained. In 1,4-dioxane solution, interestingly, complex 3 undergoes a dissolution/reorganization process to transform into 4, [Dy(bpy)(tfmb)3]·0.5C4H8O2. Structural analyses indicate that Dy(III) in 1–4 adopts an approximately square-antiprismatic (SAP) coordination environment with D4d axial symmetry. The magnetic properties of 1–4 are investigated and the M versus H data exhibit evident butterfly-shaped hysteresis loops at 2 K for 1–4. Although all the Dy(III) ions in 1–4 adopt similar configurations, their magnetization dynamics are apparently different from each other, as shown by the various heights of the effective energy barrier (Ueff) of magnetization reversal. To deeply understand their different magnetic behaviours, the magnetic anisotropy of 1–4 is systematically studied by ab initio calculations. The theoretical results further indicate that the capping ligands could play an important role in the fine tuning of the SMM property via an effect on the equatorial electrostatic potential, whereas the inclusion of guest solvent molecules could significantly influence the axial electrostatic potential, leading to a strong effect on the SMM property.read more
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Journal ArticleDOI
Experimental and Theoretical Interpretation on the Magnetic Behavior in a Series of Pentagonal-Bipyramidal DyIII Single-Ion Magnets.
Min Li,Haipeng Wu,Qi Yang,Hongshan Ke,Bing Yin,Quan Shi,Wenyuan Wang,Qing Wei,Gang Xie,Sanping Chen +9 more
TL;DR: The analysis on the electrostatic potential demonstrates that although the pentagonal bipyramidal D5h 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.
Journal ArticleDOI
3D isomorphous lanthanide coordination polymers displaying magnetic refrigeration, slow magnetic relaxation and tunable proton conduction
TL;DR: In this paper, four new isostructural lanthanide-based three-dimensional coordination polymers (CPs) have been constructed using a sulfonate-carboxylate-based ligand (Na2H2L = disodium-2,2'-disulfonate,4,4'-oxydibenzoic acid) and corresponding lanthanides metal(iii) nitrates.
Journal ArticleDOI
Manipulating the Relaxation of Quasi-D4d Dysprosium Compounds through Alternation of the O-Donor Ligands
Mei Guo,Jianfeng Wu,Jianfeng Wu,Olivier Cador,Jingjing Lu,Bing Yin,Boris Le Guennic,Jinkui Tang +7 more
TL;DR: Three mononuclear DyIII complexes with the same auxiliary ligand Lz are synthesized through alteration of the ligands containing O donors, leading to distinct magnetic properties, which were studied experimentally and via ab initio calculations.
Journal ArticleDOI
Lanthanide-Based Layer-Type Two-Dimensional Coordination Polymers Featuring Slow Magnetic Relaxation, Magnetocaloric Effect and Proton Conductivity.
TL;DR: Ab-initio calculations suggest that the g tensor of Kramers doublet of the lanthanide ion(Dy3+ and Er3+) is strongly axial in nature which reflects in slow magnetic relaxation behavior of both CPs.
Journal ArticleDOI
Single-molecule magnet behavior in a CuII-decorated {DyIII2} complex with nitronyl nitroxide biradicals
TL;DR: In this article, a novel nitronyl nitroxide biradical ligand NITPhPyoebis (1) (5-(4-pyridinone)-1,3-bis(1′-oxyl-3-oxido-4′,4-5-hydro-1H-imidazol-2-yl)benzene) was synthesized successfully.
References
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