期刊
CRYSTENGCOMM
卷 14, 期 20, 页码 7015-7024出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2ce25862e
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资金
- Grant Agency of the Czech Republic [GACR P207/11/0841]
- Operational Program Research and Development for Innovations [CZ.1.05/2.1.00/03.0058]
- Operational Program Education for Competitiveness of the Ministry of Education, Youth and Sports of the Czech Republic [CZ.1.07/2.3.00/20.0017]
- Slovak republic: VEGA [1/0052/11, APVV-0014-11]
- Germany: DAAD [ID50725741]
- Austria: Fonds zur Forderung der Wissenschaftlichen Forschung in Osterreich [19335-N17]
A series of spin crossover iron(III) complexes with the general composition [Fe(4OH-L6)]X (H-2-4OH-L6 = 1,8-bis(4-hydroxysalicylaldiminato)-3,6-diazaoctane; X = Cl, 1a; Br, 1b; I, 1c) was prepared. A combination of the results following the single crystal X-ray analysis, infrared and EPR spectroscopy, and temperature dependent magnetic experiments revealed that the Fe(III) atoms occur in the low-spin state below room temperature and the crystal structures of the complexes involve rich networks of non-covalent intermolecular contacts resulting in two-dimensional supramolecular structures. Alterations in the halide anions influence the strength of the non-covalent contacts and affect the magnetic properties of the studied complexes. The antiferromagnetic exchange interaction between the non-covalently bound cations is the most obvious in the case of 1a and it weakens with the growing anionic volume of X. The 1D and 2D spin Hamiltonian models were applied to quantitatively extract the information about the intermolecular magnetic exchange (fit on 1D infinite chain gives J(1a) = 22.86 cm(-1), J(1b) = -2.02 cm(-1), J(1c) = -1.16 cm(-1)). Furthermore, gradual spin crossover behaviour for all of the compounds of the series was observed above room temperature in the solid state. Spin crossover accompanied by thermochromism was also demonstrated by EPR experiments in solution.
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