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Pentanuclear Heterometallic {Ni2Ln3} (Ln = Gd, Dy, Tb, Ho) Assemblies. Single-molecule Magnet Behavior and Multistep Relaxation in the Dysprosium Derivative

Pentanuclear Heterometallic {Ni2Ln3} (Ln = Gd, Dy, Tb, Ho) Assemblies. Single-molecule Magnet Behavior and Multistep Relaxation in the Dysprosium Derivative

Vadapalli Chandrasekhar, Prasenjit Bag, Wolfgang Kroener, Klaus Gieb, Paul Müller

Inorg Chem. 2013 Nov 18;52(22):13078-86.

PMID: 24236759

Abstract:

The reaction between Ln(III) chloride and NiCl2·4H2O salts in presence of a multidentate sterically unencumbered ligand, (E)-2,2'-(2-hydroxy-3-((2-hydroxyphenylimino)methyl)-5-methylbenzylazanediyl)diethanol (LH4) leads to the synthesis of four isostructural pentanuclear hetereometallic complexes [Ni2Dy3(LH)4]Cl (1), [Ni2Gd3(LH)4]Cl (2), [Ni2Tb3(LH)3(LH2)]Cl2 (3), [Ni2 Ho3 (LH)3 (LH2)]Cl2 (4) with unprecedented topology. Here the two compounds 1 are 2 are monocationic and crystallize in chiral space group, P2(1)2(1)2(1) whereas compounds 3 and 4 are dicationic and crystallize in achiral space group P2(1)/n. The total metal framework, {Ni2Ln3} unit is held by four triply deprotonated ligands [LH](3-) in 1 and 2 whereas in case of 3 and 4 three triply deprotonated [LH](3-) and one doubly deprotonated [LH2](2-) ligands are involved. In these complexes both the lanthanide ions and the nickel(II) ions are doubly bridged and the bridging is composed of oxygen atoms derived from either phenolate or ethoxide groups. The analysis of SQUID measurements reveal a high magnetic ground state and a slow relaxation of the magnetization with two relaxation regimes for 1. For the thermally activated regime we found an effective energy barrier of U(eff) = 85 K. Micro Hall probe loop measurements directly proof the single-molecule magnet (SMM) nature of 1 with a blocking temperature of T(B) = 3 K and an open hysteresis for sweep rates faster than 50 mT/s.

Chemicals Related in the Paper:

Catalog Number	Product Name	Structure	CAS Number	Price
AP10025748	Dysprosium(III) chloride		10025-74-8	Price

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