期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 128, 期 14, 页码 4842-4853出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja058030v
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- ICREA Funding Source: Custom
We herein present the preparation, crystal structure, magnetic properties, and theoretical study of new heterobimetallic chains of formula {[Fe-III(bpym)(CN4)](2)M-II(H2O)(2)}center dot 6H(2)O [bpym = 2,2'-bipyrimidine; M = Zn (2), Co (3), Cu (4), and Mn (5)] which are obtained by using the building block PPh4[Fe(bpym)(CN)(4)]center dot H2O (1) (PPh4+ = tetraphenylphosphonium) as a ligand toward the fully solvated M-II ions. The structure of complex 1 contains mononuclear [Fe(bpym)(CN)(4)](-) anions. Compounds 2-5 are isostructural 4,2-ribbonlike bimetallic chains where the [Fe(bpym)(CN)(4)](-) unit acts as a bis-monodenate ligand through two of its four cyanide ligands toward the M atom. Water hexamer clusters (4) and regular alternating fused six- and four-membered water rings with two dangling water molecules (2, 3, and 5) are trapped between the cyanide-bridged 4,2-ribbonlike chains. 1 and 2 behave as magnetically isolated low-spin iron(III) centers. 3 behaves as a single-chain magnet (SCM) with intrachain ferromagnetic coupling, slow magnetic relaxation, hysteresis effects, and frequency-dependent ac signals at T < 7 K. As expected for a thermally activated process, the nucleation field (H-n) in 3 increases with decreasing T and increasing v. Below 1.0 K, H-n becomes temperature independent but remains strongly sweep rate dependent. In this temperature range, the reversal of the magnetization may be induced by a quantum nucleation of a domain wall that then propagates due to the applied field. 4 and 5 are ferro- and ferrimagnetic chains respectively, with metamagnetic-like behavior (4). DFT-type calculations and QMC methodology provided a good understanding of the magnetic properties of 3-5.
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