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As the ligand system plays the most important role in the behaviour of the spin-transition of iron(II) spin-crossover compounds a series of eight new mainly bridging di-tetrazole ligands were synthesised and produced new insights into spacer modifications as well as geometric prerequisites of the ligand and their impact on spin-crossover behaviour. The focus laid on aryl-spaced tetrazole ligands, which were interesting analogues to the well-known alkyl-di-tetrazoles due to expected enhanced interaction within the molecular structure through pi-pi-stacking. The results of this fundamental study yielded further guidelines to optimize and fine-tune the ligand design, which are envisaged to be used for spin-crossover iron(II) coordination polymers of high T1/2-values with abrupt spin transition behaviour. Additionally, one new SCO compound [mu-Tris(1-[1,1-dimethyl-2-(1H-tetrazol-1-yl)ethyl]-1H- tetrazole-N4,N4?)iron(II)] bis(tetrafluoroborate) – [Fe(dtmp) 3](BF4)2 – is presented. The compound features a spin transition around 160 K with a small thermal hysteresis of 5 K.
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