A spin crossover ferrous complex with ordered magnetic ferric anions

Roubeau, Olivier; Evangelisti, Marco; Natividad, Eva

doi:10.1039/c2cc33709f

Cited by 21 publications

(16 citation statements)

References 26 publications

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“…2 and S1, Table S3†). The similarity of these intermolecular interactions with those found in the structures of other tetrazole compounds exhibiting gradual SCO 18a,19 suggests that the cooperative hysteretic SCO in 2 is associated with the presence of crystallographic transitions ‡…”

Section: Resultssupporting

confidence: 54%

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Switchable slow relaxation of magnetization in the native low temperature phase of a cooperative spin-crossover compound

Urtizberea

Roubeau

2017

Chem. Sci.

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Section: Resultssupporting

confidence: 54%

“…In both structures, the [Fe(mtz) 6 ] 2+ cations form similar supramolecular hexagonal layers, reminiscent of analogue tetrazole complexes, 18,19 through C tz –H···A hydrogen bonds with the triflate anions (Fig. 2, Table S3†).…”

Section: Resultsmentioning

confidence: 99%

Switchable slow relaxation of magnetization in the native low temperature phase of a cooperative spin-crossover compound

Urtizberea

Roubeau

2017

Chem. Sci.

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“…The trigonal structure of 1 has one [Fe(Metz) 6 ] 2+ cation and FeBr 4 − anions building hexagonal layers extended in the ab plane (Figure 1), and pillared along the c axis, in a perfectly eclipsed conformation. According to magnetic and calorimetric measurements, [Fe(Metz) 6 ] 2+ cations present a gradual complete thermal SCO centred at 165 K, coexisting with a long range antiferromagnetic order of the FeBr 4 − anions below T N =2.4 K 19. We report here the magnetic structure of this original material and present a detailed study of how applied pressure affects both the SCO and the magnetic order.…”

Section: Introductionmentioning

confidence: 94%

“…[Fe II (Metz) 6 ](Fe III Br 4 ) 2 (Metz=1‐methyltetrazole)19 ( 1 ) is in this respect an exciting new example combining SCO and magnetic order. The trigonal structure of 1 has one [Fe(Metz) 6 ] 2+ cation and FeBr 4 − anions building hexagonal layers extended in the ab plane (Figure 1), and pillared along the c axis, in a perfectly eclipsed conformation.…”

Section: Introductionmentioning

confidence: 99%

A Multifunctional Magnetic Material under Pressure

Rodríguez-Velamazán

Fabelo

Beavers

et al. 2014

Chemistry A European J

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[Fe II (Metz)6](Fe III Br4)2 (Metz = 1-methyltetrazole) is one of the rare systems combining spincrossover and long-range magnetic ordering. The spin-crossover phenomenon of the cationic sublattice [Fe II (Metz)6] 2+ coexists in this multifunctional material with an antiferromagnetic order of the anionic sub-lattice (Fe III Br4) -. A combined study involving neutron and X-ray diffraction and bulk and single-crystal magnetometry allows determining the collinear antiferromagnetic structure of this system, and shows that the magnetic ordering is favoured by the application of pressure, with an increase of the Néel temperature from 2.4 K at ambient pressure, to 3.9 K at 0.95 GPa. Applied pressure also enables a full high-spin to low-spin switch at ambient temperature. IntroductionThe molecular approach for the design of multifunctional materials makes use of the flexibility offered by molecular systems for combining different functional properties in the same compound. Several recent examples illustrate the success of this approach, featuring e.g., magnetic and optical properties, 1 porosity and magnetism, 2 conductivity and magnetism, 3 superconductivity and magnetism, 4 or even a multiferroic character. 5 The spin crossover (SCO) phenomenon 6 is in itself a source of multifunctionality, 7 with drastic variations in magnetic, optical, dielectric and structural properties potentially taking place concomitantly with the change of spin state between high-spin (HS) and low-spin (LS) electronic configurations. 8 Conveniently, this molecular bistability can be addressed by an external perturbation 9 like temperature, 10 magnetic field, 11 light irradiation, 12 chemical stimuli 13 or pressure.14 Very recent reports have in addition shown that the light-induced HS form of an Fe(II) SCO material can behave as a Single-Molecule Magnet (SMM) and that photomagnetic chains can be designed by linking SCO and SMM building blocks. 15 On the other hand, although magnetic ordering is one of the most pursued functional properties due to its potential use in a variety of applications, 16 the molecularbased systems combining it with SCO are still scarce. This combination has been achieved in hybrid crystalline solids that integrate Fe III -anions in the unit cell, building hexagonal layers extended in the ab plane (Figure 1). These layers are pillared along the c axis, in a perfectly eclipsed conformation. According to magnetic and calorimetric measurements, [Fe(Metz)6] 2+ cations present a gradual complete thermal SCO centred at 165 K, coexisting with a long range antiferromagnetic order below TN = 2.4 K of the FeBr4 -. 19 We report here the magnetic structure of this original material and present a detailed study of how applied pressure affects both the SCO and the magnetic order. 19 We have now used powder neutron diffraction (PND) and single-crystal magnetometry for determining the magnetic structure of 1. A first high-resolution PND data collection aimed at refining the nuclear structure at low temperature has been perfo...

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“…Thus the utilization of electronic and structural transformation accompanying SCO can lead to potential applications of display, memory, sensing and electronic devices [3,4]. One of the emergent fields of SCO research in the last decade is the development of multifunctional compounds between SCO and other solid-state electronic properties such as conductivity [5][6][7][8][9][10][11][12], magnetism [13][14][15][16][17][18][19][20][21][22][23], and optical properties [24,25]. The goal of this research is that one can design and synthesize a molecular solid whose electronic property can be controlled by external stimuli.…”

Section: Introductionmentioning

confidence: 99%

Spin-Singlet Transition in the Magnetic Hybrid Compound from a Spin-Crossover Fe(III) Cation and π-Radical Anion

et al. 2017

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Abstract:To develop a new spin-crossover functional material, a magnetic hybrid compound [Fe(qsal) 2 ][Ni(mnt) 2 ] was designed and synthesized (Hqsal = N-(8-quinolyl)salicylaldimine, mnt = maleonitriledithiolate). The temperature dependence of magnetic susceptibility suggested the coexistence of the high-spin (HS) Fe(III) cation and π-radical anion at room temperature and a magnetic transition below 100 K. The thermal variation of crystal structures revealed that strong π-stacking interaction between the π-ligand in the [Fe(qsal) 2 ] cation and [Ni(mnt) 2 ] anion induced the distortion of an Fe(III) coordination structure and the suppression of a dimerization of the [Ni(mnt) 2 ] anion. Transfer integral calculations indicated that the magnetic transition below 100 K originated from a spin-singlet formation transformation in the [Ni(mnt) 2 ] dimer. The magnetic relaxation of Mössbauer spectra and large thermal variation of a g-value in electron paramagnetic resonance spectra below the magnetic transition temperature implied the existence of a magnetic correlation between d-spin and π-spin.

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A spin crossover ferrous complex with ordered magnetic ferric anions

Cited by 21 publications

References 26 publications

Switchable slow relaxation of magnetization in the native low temperature phase of a cooperative spin-crossover compound

Switchable slow relaxation of magnetization in the native low temperature phase of a cooperative spin-crossover compound

A Multifunctional Magnetic Material under Pressure

Spin-Singlet Transition in the Magnetic Hybrid Compound from a Spin-Crossover Fe(III) Cation and π-Radical Anion

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