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Three mononuclear lanthanide complexes of a 2-pyridylmethyl pendant-armed 15-membered ligand {(3,12-bis(2-pyridylmethyl)-3,12,18-triaza-6,9-dioxabicyclo-[12.3.1]octadeca-1,14,16-triene); L} with general formula [Ln(L)(H 2 O)(NO 3 )](NO 3 ) 2 (Ln = Tb (1), Dy (2), and Er (3)) are reported. Based on X-ray diffraction analysis of 1 and 2, the central lanthanide atoms are nine-coordinated with the N 5 O 4 donor set originating from the ligand L and one coordinated water molecule and one monodentate-bonded nitrato ligand. The coordination geometry of the [LnN 5 O 4 ] cores can be described as a muffin-like shape. Magnetic measurements revealed that all three compounds show field-induced single-molecule magnet behaviour, with estimated energy barriers U ≈ 44-82 K. The experimental study was complemented by CASSCF calculations showing a trend of an increasing first excited energy gap (Tb → Dy → Er) within the muffin-like geometry with the lowest magnetization tunnelling probability for the Dy III complex 2.

Muffin-like lanthanide complexes with an N5O2-donor macrocyclic ligand showing field-induced single-molecule magnet behaviour

Muffin-like lanthanide complexes with an N₅O₂-donor macrocyclic ligand showing field-induced single-molecule magnet behaviour