Abstract
Solvents play important roles in our lives, they are also of interest in molecular materials, especially for molecular magnets. The solvatomagnetic effect is generally used for trigger and/or regulation of magnetic properties in molecule-based systems, however, molecular nanomagnets showing solvatomagnetic effects are very difficult to obtain. Here we report four 3d-4f heterometallic cluster complexes containing ROH lattice solvent molecules, [Cu3Tb2(H3L)2(OAc)2(hfac)4]∙2ROH {H6L = 1,3-Bis[tris(hydroxymethyl)methylamino]propane, hfac− = hexafluoroacetylacetonate; R = CH3, 1; R = C2H5, 2; R = C3H7, 3; R = H, 4}. Single-molecule magnet (SMM) properties of these four complexes were observed to be dependent on the ROH lattice solvent molecule. There is an interesting magneto-structural correlation: the larger the R group, the higher the energy barrier. For the first time, the solvatomagnetic effect is used for the continuous fine adjustment of the energy barrier of 0D molecular nanomagnets. Additionally, [Cu3Dy2(H3L)2(OAc)2(hfac)4]∙2MeOH (5), an analogue of [Cu3Tb2(H3L)2(OAc)2(hfac)4]∙2MeOH (1), is also reported for comparison.
Highlights
It is well known that Single-molecule magnet (SMM) are of great potential for technological applications in high-density information storage, quantum computing and spintronics[12,13,14,15,16,17]; and the energy barrier leading to magnetic bistability and slow magnetic relaxation is a pivotal parameter
Murrie et al reported a series of 3d-4f complexes formulated as {Ln2Cu3(H3L)2Xn} (X = OAc−, Ln = Gd, Tb or X = NO3−, Ln = Gd, Tb, Dy, Ho, Er)[35]; they found that changing the auxiliary ligand OAc− through NO3− may lead to a remarkable improvement of the energy barrier of {Tb2Cu3(H3L)2Xn} (X = OAc− and NO3−) complexes, which suggests that the anion co-ligand has a great impact on the energy barrier of {Tb2Cu3(H3L)2Xn} SMMs
In the recent process of pursuing new SMMs, we observed that using Ln(OAc)(hfac)2(H2O)[2] as the lanthanide (III) salt source may lead mixed co-ligands OAc− and hfac− into 3d-4f heterometallic clusters effectively[36]
Summary
It is well known that SMMs are of great potential for technological applications in high-density information storage, quantum computing and spintronics[12,13,14,15,16,17]; and the energy barrier leading to magnetic bistability and slow magnetic relaxation is a pivotal parameter. Systematic studies of SMMs with the same magnetic structure are still rare, some factors such as the electron-withdrawing effect[27], the electrostatic potential of the key coordination atom[28] have been observed to be able to modulate SMMs’ energy barriers recently. To the best of our knowledge, a direct correlation between energy barriers and different lattice solvent molecules of 0D molecular nanomagnets has never been documented, though a 3D Dy(III) MOF-type SMM was found to show an obvious solvatomagnetic effect in 201529, and guest-dependent single-ion magnet behaviours were observed in a 2D cobalt(II) coordination polymer in 201630.
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