AustralieFrV1, Main, Exploration, bibRecord, 009051

Structure, magnetism and photomagnetism of mixed-ligand tris(pyrazolyl)methane iron(ii) spin crossover compounds

Identifieur interne : 009051 ( Main/Exploration ); précédent : 009050; suivant : 009052

Structure, magnetism and photomagnetism of mixed-ligand tris(pyrazolyl)methane iron(ii) spin crossover compounds

Auteurs : Boujemaa Moubaraki [Australie] ; Ben A. Leita [Australie] ; Gregory J. Halder [Australie] ; Stuart R. Batten [Australie] ; Paul Jensen [Australie] ; Jonathan P. Smith [Australie] ; John D. Cashion [Australie] ; Cameron J. Kepert [Australie] ; Jean-François Létard [France] ; Keith S. Murray [Australie]

Source :

Dalton Transactions [ 1477-9226 ] ; 2007.

RBID : ISTEX:CA38D2DC9702192B93C382BC7A8B4CD51870C4BF

English descriptors

Abstract

A range of bis-facial tridentate chelate complexes of type [Fe((R-pz)3CH)((3,5-Me2pz)3CH)](BF4)2 has been characterised that contain two different tris-pyrazolylmethane ligands, with variations in R being H (complex 1 crystallised as polymorphs 1a and 1b) and 4-Me (2), as well as R = H with a CH2OH arm off the methane carbon (3). A tris(pyridyl)methane analogue is also described (4). The tris(3,5-dimethylpyrazolyl)methane co-ligand (3,5-Me2pz), and the BF4− counterion, are constant throughout. The spin-crossover properties of these Fe(ii) d6 compounds have been probed in detail by variable temperature magnetic, Mössbauer spectral and crystallographic methods. The effects of distortions from octahedral symmetry around the Fe(ii) centres, of crystal solvate molecules (1.5 MeCN in 2 and 2 MeCN in 3) and of supramolecular/crystal packing, are discussed. In the case of 1, subtle twisting of pyrazole rings occurs, as a function of temperature, that has a greater effect upon the relative positions of the Fe(ii) chelate molecules in polymorph 1b than in polymorph 1a; this is thought to drive the cooperativity differences observed in the magnetism of the polymorphs. Comparisons are also made between 1 to 4 and their homoleptic, parent [Fe(L)2] 2+ materials. The complexes were screened for the LIESST (light induced excited spin state trapping) effect by measurements of diffuse absorption spectra on the surface of powder samples, at different temperatures. One example, 2, showed a 2-step thermal spin crossover transition and it was probed in detail for its photomagnetic features. The T(LIESST) and T1/2 values for 2 did not obey an empirical relationship, T(LIESST) = 150 − 0.3T1/2 followed by many Fe(ii)(N-donor)6 crossover compounds of the bis-tridentate (meridional) type, and possible reasons for this are discussed.

Url:

https://api.istex.fr/document/CA38D2DC9702192B93C382BC7A8B4CD51870C4BF/fulltext/pdf

DOI: 10.1039/b708773j

Affiliations:

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Le document en format XML

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<term>Block triclinic</term>
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<term>Colourless crystals</term>
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<term>Crystal data</term>
<term>Crystallographic data</term>
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<term>Data integration</term>
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<term>Diffuse absorption spectra</term>
<term>Distance distance</term>
<term>Distortion angle</term>
<term>Donor plane</term>
<term>Doublet</term>
<term>Empirical relationship</term>
<term>Formula crystal colour</term>
<term>Further details</term>
<term>Further work</term>
<term>Gradual crossover</term>
<term>Higher temperature</term>
<term>Hydrogen atoms</term>
<term>Hysteresis</term>
<term>Infrared spectrum</term>
<term>Inorg</term>
<term>Intermolecular interactions</term>
<term>Irreg</term>
<term>Latter forms</term>
<term>Liesst</term>
<term>Liesst effect</term>
<term>Liesst phenomenon</term>
<term>Liesst properties</term>
<term>Ligand</term>
<term>Magnetic data</term>
<term>Magnetic moment</term>
<term>Mecn</term>
<term>Meridional tridentate</term>
<term>Metal atoms</term>
<term>Mmol</term>
<term>Mole equivalent</term>
<term>Molecular reorganisation</term>
<term>Monash university</term>
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<term>Mossbauer spectra</term>
<term>Mossbauer spectrum</term>
<term>Octahedral</term>
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<term>Photomagnetic measurements</term>
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<term>Physical measurements</term>
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<term>Reger</term>
<term>Room temperature</term>
<term>Royal society</term>
<term>Same level</term>
<term>Side angle</term>
<term>Solvate</term>
<term>Squid magnetometer</term>
<term>Structural features</term>
<term>Such interactions</term>
<term>Tard</term>
<term>Temperature dependence</term>
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<term>Thin layer</term>
<term>Total signal</term>
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<term>Transition temperature</term>
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<term>Tridentate</term>
<term>Tridentate ligands</term>
<term>Trigonal angles</term>
<term>Unique data</term>
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<term>Whole range</term>
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<term>Anion</term>
<term>Block triclinic</term>
<term>Bond angles</term>
<term>Bond lengths</term>
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<term>Chem</term>
<term>Colourless</term>
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<term>Crystallographic data</term>
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<term>Data integration</term>
<term>Different temperatures</term>
<term>Diffuse absorption spectra</term>
<term>Distance distance</term>
<term>Distortion angle</term>
<term>Donor plane</term>
<term>Doublet</term>
<term>Empirical relationship</term>
<term>Formula crystal colour</term>
<term>Further details</term>
<term>Further work</term>
<term>Gradual crossover</term>
<term>Higher temperature</term>
<term>Hydrogen atoms</term>
<term>Hysteresis</term>
<term>Infrared spectrum</term>
<term>Inorg</term>
<term>Intermolecular interactions</term>
<term>Irreg</term>
<term>Latter forms</term>
<term>Liesst</term>
<term>Liesst effect</term>
<term>Liesst phenomenon</term>
<term>Liesst properties</term>
<term>Ligand</term>
<term>Magnetic data</term>
<term>Magnetic moment</term>
<term>Mecn</term>
<term>Meridional tridentate</term>
<term>Metal atoms</term>
<term>Mmol</term>
<term>Mole equivalent</term>
<term>Molecular reorganisation</term>
<term>Monash university</term>
<term>Mossbauer</term>
<term>Mossbauer spectra</term>
<term>Mossbauer spectrum</term>
<term>Octahedral</term>
<term>Octahedral geometry</term>
<term>Octahedral symmetry</term>
<term>Phase change</term>
<term>Photomagnetic</term>
<term>Photomagnetic measurements</term>
<term>Phys</term>
<term>Physical measurements</term>
<term>Pink crystals</term>
<term>Pink solution</term>
<term>Polymorph</term>
<term>Pyrazole rings</term>
<term>Pyrazolyl rings</term>
<term>Quadrupole doublet</term>
<term>Reger</term>
<term>Room temperature</term>
<term>Royal society</term>
<term>Same level</term>
<term>Side angle</term>
<term>Solvate</term>
<term>Squid magnetometer</term>
<term>Structural features</term>
<term>Such interactions</term>
<term>Tard</term>
<term>Temperature dependence</term>
<term>Thermal hysteresis</term>
<term>Thin layer</term>
<term>Total signal</term>
<term>Trans</term>
<term>Transition temperature</term>
<term>Triclinic</term>
<term>Tridentate</term>
<term>Tridentate ligands</term>
<term>Trigonal angles</term>
<term>Unique data</term>
<term>Unit cell angles</term>
<term>Unit cell parameters</term>
<term>Unit cell volume</term>
<term>Volume changes</term>
<term>Whole range</term>
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<front><div type="abstract">A range of bis-facial tridentate chelate complexes of type [Fe((R-pz)3CH)((3,5-Me2pz)3CH)](BF4)2 has been characterised that contain two different tris-pyrazolylmethane ligands, with variations in R being H (complex 1 crystallised as polymorphs 1a and 1b) and 4-Me (2), as well as R = H with a CH2OH arm off the methane carbon (3). A tris(pyridyl)methane analogue is also described (4). The tris(3,5-dimethylpyrazolyl)methane co-ligand (3,5-Me2pz), and the BF4− counterion, are constant throughout. The spin-crossover properties of these Fe(ii) d6 compounds have been probed in detail by variable temperature magnetic, Mössbauer spectral and crystallographic methods. The effects of distortions from octahedral symmetry around the Fe(ii) centres, of crystal solvate molecules (1.5 MeCN in 2 and 2 MeCN in 3) and of supramolecular/crystal packing, are discussed. In the case of 1, subtle twisting of pyrazole rings occurs, as a function of temperature, that has a greater effect upon the relative positions of the Fe(ii) chelate molecules in polymorph 1b than in polymorph 1a; this is thought to drive the cooperativity differences observed in the magnetism of the polymorphs. Comparisons are also made between 1 to 4 and their homoleptic, parent [Fe(L)2] 2+ materials. The complexes were screened for the LIESST (light induced excited spin state trapping) effect by measurements of diffuse absorption spectra on the surface of powder samples, at different temperatures. One example, 2, showed a 2-step thermal spin crossover transition and it was probed in detail for its photomagnetic features. The T(LIESST) and T1/2 values for 2 did not obey an empirical relationship, T(LIESST) = 150 − 0.3T1/2 followed by many Fe(ii)(N-donor)6 crossover compounds of the bis-tridentate (meridional) type, and possible reasons for this are discussed.</div>
</front>
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Serveur d'exploration sur les relations entre la France et l'Australie

Structure, magnetism and photomagnetism of mixed-ligand tris(pyrazolyl)methane iron(ii) spin crossover compounds

Structure, magnetism and photomagnetism of mixed-ligand tris(pyrazolyl)methane iron(ii) spin crossover compounds

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