Abstract
Exploring the chemistry of vanadyl ions (VO2+) with bis-β-diketone ligands, in pyridine reactions of vanadyl sulfate with 1,3-bis-(3-oxo-3-(2-hydroxyphenyl)-propionyl)-benzene (H4L1) and 1,3-bis-(3-oxo-3-(2-hydroxyphenyl)-propionyl)-pyridine (H4L2), two novel clusters, [(VIVO)4(H2L1)4(py)4] (1) and [(VVO)4(VIVO)2 (O)4(L2)2(py)6] (2) were prepared and characterized. Due to the conformational flexibility of the ligands, both entities exhibit very peculiar metal topologies and composition, differing significantly from structural patterns established in the related chemistry of divalent 3d metals. Structural analysis also unveils the existence of the most complex metallamacrocycles from this family to date. Studies of the magnetic properties via bulk magnetization measurements and EPR spectroscopy confirmed the existence of uncoupled long-distant S = 1/2 metal centers and the spin ground states S = 2 and S = 1 of the clusters.
Highlights
The field of molecular magnetism has illuminated the discovery of magnetic functional systems of molecular bases, such as single molecule magnets (SMMs) [1,2,3,4,5], bi-stable spin crossover (SCO)materials [6,7,8], or proposed molecular hardware for spin-based quantum computing (QC) [9,10,11,12]
The structural versatility of H4L1 and H4L2 has been emphasized in the Introduction
The former donor has allowed the subtle control of cluster topology and nuclearity [19,40,42], whereas the latter led to the discovery of unexpected structural features [27,28]
Summary
The field of molecular magnetism has illuminated the discovery of magnetic functional systems of molecular bases, such as single molecule magnets (SMMs) [1,2,3,4,5], bi-stable spin crossover (SCO). Materials [6,7,8], or proposed molecular hardware for spin-based quantum computing (QC) [9,10,11,12] In this endeavor, the field of coordination chemistry is an inexhaustible spring of tools resulting from the combination of versatile organic scaffolds and the diverse physico-chemical properties of transition and rare-earth metals. The field of coordination chemistry is an inexhaustible spring of tools resulting from the combination of versatile organic scaffolds and the diverse physico-chemical properties of transition and rare-earth metals In this context, the implementation of judiciously engineered ligands, such as bis-β-diketones [13], has allowed the preparation of abundant families of metallohelicates [14,15,16], linear molecular platforms [17,18], weakly coupled molecular cluster pairs [19,20], metallamacrocycles [21,22,23,24], and cage clusters [25,26,27,28] displaying interesting topologies and unprecedented structural features.
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