Rare “Janus”-faced  single-molecule magnet exhibiting intramolecular ferromagnetic interactions

Alexandropoulos, Dimitris I.; Vignesh, Kuduva R.; Stamatatos, Theocharis C.; Dunbar, Kim R.

doi:10.1039/c8sc04384a

Cited by 28 publications

(15 citation statements)

References 64 publications

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“…Finally, the χ M T values rapidly increased to 98.6 and 137.2 cm 3 K mol −1 for 2 and 4 at 2 K, respectively, which may have resulted from the weak ferromagnetic interactions in the temperature range of 2−10 K. 23 For 3, the χ M T values remained almost constant in the temperature range of 300−20 K but then rapidly decreased to a value of 38.9 cm 3 K mol −1 as the temperature was decreased to 2 K, suggesting that there were weak paramagnetic interactions in the high temperature range and significant zero-field splitting and weak antiferromagnetic intermolecular interactions in the low temperature zone. 24 It is crucial to fully understand the magnetic interaction between metals to improve the MCE of the molecular magnetism. Therefore, based on the Algorithms and Libraries for Physical Simulations (ALPS) 25 project, the Quantum Monte Carlo (QMC) calculation method was performed to fit the value of χ M T vs T and calculate the magnetic coupling interaction.…”

Section: Resultsmentioning

confidence: 99%

Anion-Dependent Assembly of 3d–4f Heterometallic Clusters Ln₅Cr₂ and Ln₈Cr₄

et al. 2020

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A series of heterometallic Ln–Cr clusters with the formulas [Ln5Cr2(H2L)2(OAc)6(μ3-OH)6(H2O)15](ClO4)7·xH2O (Ln = Gd and x = 33 for 1 and Ln = Dy and x = 21 for 2) and [Ln8Cr4(H2L)4(OAc)8(μ3-OH)16(μ4-O)1(H2O)8](Cl)(ClO4)5·10H2O (Ln = Gd for 3 and Ln = Dy for 4) was obtained through the reaction of the acetate ligands 2,2-dimethylolpropionic acid (H3L) and Ln(ClO4)3 in the presence of chromium salts with different anions under the same high pH conditions. X-ray analysis revealed that compound 1 contained a metal unit [Gd3Cr2] displaying the pentagonal bipyramid configuration and that compound 3 was templated by Cl– and ClO4 – as a mixed anion template featuring a quadrangular structure. In compound 3, the 12 metal atoms were arranged in a wheel-shaped metal skeleton [Gd8Cr4], which was produced by 4 tetrahedral metal units [Gd3Cr] sharing vertices. The introduction of the mixed anion template increased the number of metal atoms in the Ln–Cr clusters. Magnetic calculations indicated that there was weak antiferromagnetic Gd···Cr coupling and weak ferromagnetic Gd···Gd coupling in 1, whereas both Gd···Cr and Gd···Gd in 3 exhibited weak antiferromagnetic interactions. Magnetothermal studies showed that compounds 1 and 3 displayed magnetic entropy changes of 25.2 J kg–1 K–1 at 5 K and 7 T and 33.8 J kg–1 K–1 at 2 K and 7 T, respectively.

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Section: Resultsmentioning

confidence: 99%

Anion-Dependent Assembly of 3d–4f Heterometallic Clusters Ln₅Cr₂ and Ln₈Cr₄

et al. 2020

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“…In those moleculars pecies, the organic moieties (ligands) are carefully chosen to predictably modulate the physical properties of the final compound. [12][13][14] However,s erendipitous transformationo ft he ligandm ight occur upon interaction with the metal centre. This is well highlighted in the family of 1,2,4,5-tetrazine-based ligands.…”

Section: Introductionmentioning

confidence: 99%

Asymmetric Ring Opening in a Tetrazine‐Based Ligand Affords a Tetranuclear Opto‐Magnetic Ytterbium Complex

Richardson

Marin

Zhang

et al. 2020

Chemistry A European J

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We report the formation of a tetranuclear lanthanide cluster, [Yb4(bpzch)2(fod)10] (1), which occurs from a serendipitous ring opening of the functionalised tetrazine bridging ligand, bpztz (3,6‐dipyrazin‐2‐yl‐1,2,4,5‐tetrazine) upon reacting with Yb(fod)3 (fod−=6,6,7,7,8,8,8‐heptafluoro‐2,2‐dimethyl‐3,5‐octandionate). Compound 1 was structurally elucidated via single‐crystal X‐ray crystallography and subsequently magnetically and spectroscopically characterised to analyse its magnetisation dynamics and its luminescence behaviour. Computational studies validate the observed MJ energy levels attained by spectroscopy and provides a clearer picture of the slow relaxation of the magnetisation dynamics and relaxation pathways. These studies demonstrate that 1 acts as a single‐molecule magnet (SMM) under an applied magnetic field in which the relaxation occurs via a combination of Raman, direct, and quantum tunnelling processes, a behaviour further rationalised analysing the luminescent properties. This marks the first lanthanide‐containing molecule that forms by means of an asymmetric tetrazine decomposition.

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“…Such compounds often exhibit interesting magnetic properties, which underlie spintronic elements and quantum devices . Although single molecule magnets were found to show ferromagnetism only at low temperatures, − some organic molecular crystals (which may be chiral , ), as well as some paramagnetic and diamagnetic organic molecules assembled in supramolecular structures, , reveal ambient temperature ferromagnetism. − For example, the assembly of hexacyanoferrate(III) anions and nickel(II) bisdiamino complexes of the chiral ligand trans -cyclohexane-1,2-diamine yields cyanide-bridged two-dimensional ferromagnets. Their crystal structure is built from cyanide-bridged bimetallic planes separated by bulky ligands.…”

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Long-Range Spin-Selective Transport in Chiral Metal–Organic Crystals with Temperature-Activated Magnetization

et al. 2020

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Room-temperature, long-range (300 nm), chirality-induced spin-selective electron conduction is found in chiral metal–organic Cu(II) phenylalanine crystals, using magnetic conductive-probe atomic force microscopy. These crystals are found to be also weakly ferromagnetic and ferroelectric. Notably, the observed ferromagnetism is thermally activated, so that the crystals are antiferromagnetic at low temperatures and become ferromagnetic above ∼50 K. Electron paramagnetic resonance measurements and density functional theory calculations suggest that these unusual magnetic properties result from indirect exchange interaction of the Cu(II) ions through the chiral lattice.

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Rare “Janus”-faced single-molecule magnet exhibiting intramolecular ferromagnetic interactions

Abstract: The unusual ferromagnetically coupled compound was prepared by the use of Me3SiN3 with the metal ions being exclusively bridged by end-on N3−. Th cationic molecule is a rare example of a 3d-metal cluster exhibiting a “Janus”-faced SMM behavior for the dried and wet forms.

Cited by 28 publications

References 64 publications

Anion-Dependent Assembly of 3d–4f Heterometallic Clusters Ln₅Cr₂ and Ln₈Cr₄

Anion-Dependent Assembly of 3d–4f Heterometallic Clusters Ln₅Cr₂ and Ln₈Cr₄

Asymmetric Ring Opening in a Tetrazine‐Based Ligand Affords a Tetranuclear Opto‐Magnetic Ytterbium Complex

Long-Range Spin-Selective Transport in Chiral Metal–Organic Crystals with Temperature-Activated Magnetization

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Rare “Janus”-faced single-molecule magnet exhibiting intramolecular ferromagnetic interactions

Abstract: The unusual ferromagnetically coupled compound was prepared by the use of Me3SiN3 with the metal ions being exclusively bridged by end-on N3−. Th cationic molecule is a rare example of a 3d-metal cluster exhibiting a “Janus”-faced SMM behavior for the dried and wet forms.

Cited by 28 publications

References 64 publications

Anion-Dependent Assembly of 3d–4f Heterometallic Clusters Ln5Cr2 and Ln8Cr4

Anion-Dependent Assembly of 3d–4f Heterometallic Clusters Ln5Cr2 and Ln8Cr4

Asymmetric Ring Opening in a Tetrazine‐Based Ligand Affords a Tetranuclear Opto‐Magnetic Ytterbium Complex

Long-Range Spin-Selective Transport in Chiral Metal–Organic Crystals with Temperature-Activated Magnetization

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Anion-Dependent Assembly of 3d–4f Heterometallic Clusters Ln₅Cr₂ and Ln₈Cr₄

Anion-Dependent Assembly of 3d–4f Heterometallic Clusters Ln₅Cr₂ and Ln₈Cr₄