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• W2131120338 abstract "Abstract Three iron(II) complexes, [Fe(TPMA)(BIM)](ClO 4 ) 2 ⋅0.5H 2 O ( 1 ), [Fe(TPMA)(XBIM)](ClO 4 ) 2 ( 2 ), and [Fe(TPMA)(XBBIM)](ClO 4 ) 2 ⋅0.75CH 3 OH ( 3 ), were prepared by reactions of Fe II perchlorate and the corresponding ligands (TPMA=tris(2‐pyridylmethyl)amine, BIM=2,2′‐biimidazole, XBIM=1,1′‐(α,α′‐ o ‐xylyl)‐2,2′‐biimidazole, XBBIM=1,1′‐(α,α′‐ o ‐xylyl)‐2,2′‐bibenzimidazole). The compounds were investigated by a combination of X‐ray crystallography, magnetic and photomagnetic measurements, and Mössbauer and optical absorption spectroscopy. Complex 1 exhibits a gradual spin crossover (SCO) with T 1/2 =190 K, whereas 2 exhibits an abrupt SCO with approximately 7 K thermal hysteresis ( T 1/2 =196 K on cooling and 203 K on heating). Complex 3 is in the high‐spin state in the 2–300 K range. The difference in the magnetic behavior was traced to differences between the inter‐ and intramolecular interactions in 1 and 2 . The crystal packing of 2 features a hierarchy of intermolecular interactions that result in increased cooperativity and abruptness of the spin transition. In 3 , steric repulsion between H atoms of one of the pyridyl substituents of TPMA and one of the benzene rings of XBBIM results in a strong distortion of the Fe II coordination environment, which stabilizes the high‐spin state of the complex. Both 1 and 2 exhibit a photoinduced low‐spin to high‐spin transition (LIESST effect) at 5 K. The difference in the character of intermolecular interactions of 1 and 2 also manifests in the kinetics of the decay of the photoinduced high‐spin state. For 1 , the decay rate constant follows the single‐exponential law, whereas for 2 it is a stretched exponential, reflecting the hierarchical nature of intermolecular contacts. The structural parameters of the photoinduced high‐spin state at 50 K are similar to those determined for the high‐spin state at 295 K. This study shows that N ‐alkylation of BIM has a negligible effect on the ligand field strength. Therefore, the combination of TPMA and BIM offers a promising ligand platform for the design of functionalized SCO complexes." @default.
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• W2131120338 date "2012-10-15" @default.
• W2131120338 modified "2023-10-18" @default.
• W2131120338 title "Heteroleptic Fe^IIComplexes of 2,2′-Biimidazole and Its Alkylated Derivatives: Spin-Crossover and Photomagnetic Behavior" @default.
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• W2131120338 doi "https://doi.org/10.1002/chem.201202045" @default.
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