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The design and synthesis of a Schiff base H 2 L, (2-{[(2-hydroxy-3-methoxybenzyl)imino]methyl}phenol), bearing an ONOO donor set has been explored for its reactivity pattern with LnCl 3 ·6H 2 O (Ln = Gd III and Dy III ) and Ni(CH 3 CO 2 ) 2 ·4H 2 O in the presence of NE 3 for molecular aggregation. Coordination driven spontaneous self-assembly reactions provide [Gd 2 Ni 6 L 4 (μ 3 -OH) 6 (μ-OH) 2 (CH 3 CO 2 ) 2 (μ-H 2 O) 2 (H 2 O) 3 (MeOH)]·8H 2 O (1) having a 'butterfly-shaped' core and [Dy 2 Ni 6 L 4 (μ 3 -OH) 4 (μ-Cl) 2 Cl 4 (H 2 O) 2 (MeOH) 2 ]·2MeOH·4H 2 O (2) with a 'candy-shaped' core. Fusion of six partial cubane units led to a mineral-like core in 1, developed around the central Ni 2 (OH) 2 moiety, whereas in the case of 2, four such partial cubanes collapsed on Dy 2 (OH) 2 . Direct-current (dc) magnetic susceptibility measurements revealed that predominant ferromagnetic interactions lead to a high-spin S = 13 ground state for 1. Complex 2 exhibits slow relaxation of magnetization under an applied small dc field with an energy barrier to reorientation of the magnetization, U eff = 19.3 K. The static and dynamic magnetic data are analysed and corroborated by density functional theory (DFT) and detailed CASSCF based calculations.

dalton transactions

Hydroxido supported and differently networked octanuclear Ni6Ln2 [Ln = GdIII and DyIII] complexes: structural variation, magnetic properties and theoretical insights