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Lanthanide cryptate monometallic coordination complexes
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DOI：10.1039/d0dt02448a.png)
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Abstract
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We report the synthesis, characterisation and magnetic properties of six novel neutral lanthanide cryptate coordination complexes. Reaction of 2,6-diformyl-4-methylphenol, tris(2-aminoethyl)amine and Ln(OTf)(3)center dot 9H(2)O in the ratio 3 : 2 :1, respectively, and in the presence of base affords the isolation of the six complexes LnL center dot 4H(2)O (Ln = Tb (1), Dy (2), Ho (3), Er (4), Tm (5) and Yb (6)), with H3L being the cryptand N[(CH2)(2)N = CH-R-CH N-(CH2)(2)](3)N (R = m-C6H2OH-2-Me-5). Powder X-ray diffraction confirms that the six complexes are isostructural. The crystal structure of 6 reveals that the Ln(iii) centre is heptacoordinated, in a geometry close to a monocapped distorted octahedron and lies on a pseudo (non-crystallo-graphically imposed) C3 axis. This coordination sphere is similar to the one found in the previously studied Ln(trensal) complexes (H(3)trensal = 2,2',2 ''-tris(salicylideneimino)triethylamine). The static and dynamic magnetic properties of these complexes were investigated by SQUID magnetometry. Crystal field parameters were determined for all complexes by modelling of the direct current magnetic susceptibility and variable-temperature-variable-field magnetisation data. As for Ln(trensal), only complexes containing the Kramers ions Dy, Er and Yb displayed out-of-phase susceptibility signals in SQUID measurements in an applied magnetic field. Investigation of the dynamic susceptibility of the Yb complex revealed that the magnetic relaxation is governed by a direct process at low temperatures and a Raman process at higher temperatures, similar to Yb(trensal).
Keywords:
SINGLE-MOLECULE MAGNETS
SPIN-LATTICE-RELAXATION
LIGAND-FIELD ANALYSIS
ANISOTROPY BARRIER
STRUCTURAL-CHARACTERIZATION
QUANTUM COHERENCE
CRYSTAL-STRUCTURE
MAGNETIZATION
QUBITS
OSCILLATIONS
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