A New Family of Spin Crossover Complexes with a Tripod Ligand Containing Three Imidazoles (see abstract)

Yuichi Ikuta, Makoto Ooidemizu, Yuichi Yamahata, Masahiro Yamada, Shutaro Osa, Naohide Matsumoto, Seiichiro Iijima, Yukinari Sunatsuki, Masaaki Kojima, Françoise Dahan, Jean Pierre Tuchagues

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Abstract

A new family of spin crossover complexes, [FeIIH 3LMe](NO3)2·1.5H 2O (1), [FeIIILMe]·3.5H2O (2), [FeIIH3LMe][FeIIL Me]NO3 (3), and [FeIIH3L Me][FeIIILMe]NO3)2 (4), has been synthesized and characterized, where H3LMe denotes a hexadentate N6 tripod ligand containing three imidazole groups, tris[2-(((2-methylimidazol-4-yl)methylidene)amino)ethyl]amine). It was found that the spin and oxidation states of the iron complexes with this tripod ligand are tuned by the degree of deprotonation of the imidazole groups and by the 2-methyl imidazole substituent. Magnetic susceptibility and Mössbauer studies revealed that 1 is an HS-FeII complex, 2 exhibits a spin equilibrium between HS and LS-FeIII, 3 exhibits a two-step spin transition, where the component [FeIILMe]- with the deprotonated ligand participates in the spin transition process in the higher temperature range and the component [FeIIH3L Me]2+ with the neutral ligand participates in the spin transition process in the lower temperature range, and 4 exhibits spin transition of both the FeII and FeIII sites. The crystal structure of 3 consists of homochiral extended 2D puckered sheets, in which the capped tripodlike components [FeIIH3LMe] 2+ and [FeIILMe]- are alternately arrayed in an up-and-down mode and are linked by the imidazole-imidazolate hydrogen bonds. Furthermore, the adjacent 2D homochiral sheets are stacked in the crystal lattice yielding a conglomerate as confirmed by the enantiomeric circular dichorism spectra. Compounds 3 and 4 showed the LIESST (light induced excited spin state trapping) and reverse-LIESST effects upon irradiation with green and red light, respectively.

Original languageEnglish
Pages (from-to)7001-7017
Number of pages17
JournalInorganic Chemistry
Volume42
Issue number22
DOIs
Publication statusPublished - Nov 3 2003

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Imidazoles
tripods
imidazoles
crossovers
Ligands
ligands
Deprotonation
Magnetic susceptibility
Crystal lattices
Hydrogen bonds
Iron
Crystal structure
Irradiation
trapping
Oxidation
Temperature
imidazole
crystal lattices
amines
hydrogen bonds

ASJC Scopus subject areas

  • Inorganic Chemistry

Cite this

Ikuta, Y., Ooidemizu, M., Yamahata, Y., Yamada, M., Osa, S., Matsumoto, N., ... Tuchagues, J. P. (2003). A New Family of Spin Crossover Complexes with a Tripod Ligand Containing Three Imidazoles (see abstract). Inorganic Chemistry, 42(22), 7001-7017. https://doi.org/10.1021/ic034495f

A New Family of Spin Crossover Complexes with a Tripod Ligand Containing Three Imidazoles (see abstract). / Ikuta, Yuichi; Ooidemizu, Makoto; Yamahata, Yuichi; Yamada, Masahiro; Osa, Shutaro; Matsumoto, Naohide; Iijima, Seiichiro; Sunatsuki, Yukinari; Kojima, Masaaki; Dahan, Françoise; Tuchagues, Jean Pierre.

In: Inorganic Chemistry, Vol. 42, No. 22, 03.11.2003, p. 7001-7017.

Research output: Contribution to journalArticle

Ikuta, Y, Ooidemizu, M, Yamahata, Y, Yamada, M, Osa, S, Matsumoto, N, Iijima, S, Sunatsuki, Y, Kojima, M, Dahan, F & Tuchagues, JP 2003, 'A New Family of Spin Crossover Complexes with a Tripod Ligand Containing Three Imidazoles (see abstract)', Inorganic Chemistry, vol. 42, no. 22, pp. 7001-7017. https://doi.org/10.1021/ic034495f
Ikuta, Yuichi ; Ooidemizu, Makoto ; Yamahata, Yuichi ; Yamada, Masahiro ; Osa, Shutaro ; Matsumoto, Naohide ; Iijima, Seiichiro ; Sunatsuki, Yukinari ; Kojima, Masaaki ; Dahan, Françoise ; Tuchagues, Jean Pierre. / A New Family of Spin Crossover Complexes with a Tripod Ligand Containing Three Imidazoles (see abstract). In: Inorganic Chemistry. 2003 ; Vol. 42, No. 22. pp. 7001-7017.
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abstract = "A new family of spin crossover complexes, [FeIIH 3LMe](NO3)2·1.5H 2O (1), [FeIIILMe]·3.5H2O (2), [FeIIH3LMe][FeIIL Me]NO3 (3), and [FeIIH3L Me][FeIIILMe]NO3)2 (4), has been synthesized and characterized, where H3LMe denotes a hexadentate N6 tripod ligand containing three imidazole groups, tris[2-(((2-methylimidazol-4-yl)methylidene)amino)ethyl]amine). It was found that the spin and oxidation states of the iron complexes with this tripod ligand are tuned by the degree of deprotonation of the imidazole groups and by the 2-methyl imidazole substituent. Magnetic susceptibility and M{\"o}ssbauer studies revealed that 1 is an HS-FeII complex, 2 exhibits a spin equilibrium between HS and LS-FeIII, 3 exhibits a two-step spin transition, where the component [FeIILMe]- with the deprotonated ligand participates in the spin transition process in the higher temperature range and the component [FeIIH3L Me]2+ with the neutral ligand participates in the spin transition process in the lower temperature range, and 4 exhibits spin transition of both the FeII and FeIII sites. The crystal structure of 3 consists of homochiral extended 2D puckered sheets, in which the capped tripodlike components [FeIIH3LMe] 2+ and [FeIILMe]- are alternately arrayed in an up-and-down mode and are linked by the imidazole-imidazolate hydrogen bonds. Furthermore, the adjacent 2D homochiral sheets are stacked in the crystal lattice yielding a conglomerate as confirmed by the enantiomeric circular dichorism spectra. Compounds 3 and 4 showed the LIESST (light induced excited spin state trapping) and reverse-LIESST effects upon irradiation with green and red light, respectively.",
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T1 - A New Family of Spin Crossover Complexes with a Tripod Ligand Containing Three Imidazoles (see abstract)

AU - Ikuta, Yuichi

AU - Ooidemizu, Makoto

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AU - Yamada, Masahiro

AU - Osa, Shutaro

AU - Matsumoto, Naohide

AU - Iijima, Seiichiro

AU - Sunatsuki, Yukinari

AU - Kojima, Masaaki

AU - Dahan, Françoise

AU - Tuchagues, Jean Pierre

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N2 - A new family of spin crossover complexes, [FeIIH 3LMe](NO3)2·1.5H 2O (1), [FeIIILMe]·3.5H2O (2), [FeIIH3LMe][FeIIL Me]NO3 (3), and [FeIIH3L Me][FeIIILMe]NO3)2 (4), has been synthesized and characterized, where H3LMe denotes a hexadentate N6 tripod ligand containing three imidazole groups, tris[2-(((2-methylimidazol-4-yl)methylidene)amino)ethyl]amine). It was found that the spin and oxidation states of the iron complexes with this tripod ligand are tuned by the degree of deprotonation of the imidazole groups and by the 2-methyl imidazole substituent. Magnetic susceptibility and Mössbauer studies revealed that 1 is an HS-FeII complex, 2 exhibits a spin equilibrium between HS and LS-FeIII, 3 exhibits a two-step spin transition, where the component [FeIILMe]- with the deprotonated ligand participates in the spin transition process in the higher temperature range and the component [FeIIH3L Me]2+ with the neutral ligand participates in the spin transition process in the lower temperature range, and 4 exhibits spin transition of both the FeII and FeIII sites. The crystal structure of 3 consists of homochiral extended 2D puckered sheets, in which the capped tripodlike components [FeIIH3LMe] 2+ and [FeIILMe]- are alternately arrayed in an up-and-down mode and are linked by the imidazole-imidazolate hydrogen bonds. Furthermore, the adjacent 2D homochiral sheets are stacked in the crystal lattice yielding a conglomerate as confirmed by the enantiomeric circular dichorism spectra. Compounds 3 and 4 showed the LIESST (light induced excited spin state trapping) and reverse-LIESST effects upon irradiation with green and red light, respectively.

AB - A new family of spin crossover complexes, [FeIIH 3LMe](NO3)2·1.5H 2O (1), [FeIIILMe]·3.5H2O (2), [FeIIH3LMe][FeIIL Me]NO3 (3), and [FeIIH3L Me][FeIIILMe]NO3)2 (4), has been synthesized and characterized, where H3LMe denotes a hexadentate N6 tripod ligand containing three imidazole groups, tris[2-(((2-methylimidazol-4-yl)methylidene)amino)ethyl]amine). It was found that the spin and oxidation states of the iron complexes with this tripod ligand are tuned by the degree of deprotonation of the imidazole groups and by the 2-methyl imidazole substituent. Magnetic susceptibility and Mössbauer studies revealed that 1 is an HS-FeII complex, 2 exhibits a spin equilibrium between HS and LS-FeIII, 3 exhibits a two-step spin transition, where the component [FeIILMe]- with the deprotonated ligand participates in the spin transition process in the higher temperature range and the component [FeIIH3L Me]2+ with the neutral ligand participates in the spin transition process in the lower temperature range, and 4 exhibits spin transition of both the FeII and FeIII sites. The crystal structure of 3 consists of homochiral extended 2D puckered sheets, in which the capped tripodlike components [FeIIH3LMe] 2+ and [FeIILMe]- are alternately arrayed in an up-and-down mode and are linked by the imidazole-imidazolate hydrogen bonds. Furthermore, the adjacent 2D homochiral sheets are stacked in the crystal lattice yielding a conglomerate as confirmed by the enantiomeric circular dichorism spectra. Compounds 3 and 4 showed the LIESST (light induced excited spin state trapping) and reverse-LIESST effects upon irradiation with green and red light, respectively.

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