A Bell-Shaped Mn<sub>11</sub>Gd<sub>2</sub> Single-Molecule Magnet

Mereacre, Valeriu; Ako, Ayuk M.; Clérac, Rodolphe; Wernsdorfer, Wolfgang; Filoti, G.; Bartolomé, J.; Anson, Christopher E.; Powell, Annie K.

doi:10.1021/ja071073m

Cited by 292 publications

(74 citation statements)

References 18 publications

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“…Finding Recent research by us and others into mixed 3d/4f systems [9][10][11] offers various means to increase both spin and total anisotropy. En route we synthesised the Gd-containing isotropic member of a new series of cyclic CCs [Fe 10 Ln 10 (Me-tea) 10 (Me-teaH) 10 (2).…”

Section: Introductionmentioning

confidence: 99%

High spin cycles: topping the spin record for a single molecule verging on quantum criticality

et al. 2018

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The cyclisation of a short chain into a ring provides fascinating scenarios in terms of transforming a finite array of spins into a quasiinfinite structure. If frustration is present, theory predicts interesting quantum critical points, where the ground state and thus lowtemperature properties of a material change drastically upon even a small variation of appropriate external parameters. This can be visualised as achieving a very high and pointed summit where the way down has an infinity of possibilities, which by any parameter change will be rapidly chosen, in order to reach the final ground state. Here we report a mixed 3d/4f cyclic coordination cluster that turns out to be very near or even at such a quantum critical point. It has a ground state spin of S = 60, the largest ever observed for a molecule (120 times that of a single electron). [Fe 10 Gd 10 (Me-tea) 10 (Me-teaH) 10 (NO 3 ) 10 ]·20MeCN forms a nano-torus with alternating gadolinium and iron ions with a nearest neighbour Fe-Gd coupling and a frustrating next-nearest neighbour Fe-Fe coupling. Such a spin arrangement corresponds to a cyclic delta or saw-tooth chain, which can exhibit unusual frustration effects. In the present case, the quantum critical point bears a 'flatland' of tens of thousands of energetically degenerate states between which transitions are possible at no energy costs with profound caloric consequences. Entropy-wise the energy flatland translates into the pointed summit overlooking the entropy landscape. Going downhill several target states can be reached depending on the applied physical procedure which offers new prospects for addressability.

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Section: Introductionmentioning

confidence: 99%

High spin cycles: topping the spin record for a single molecule verging on quantum criticality

et al. 2018

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“…[6][7][8][9] The synthesis of molecules combining the magnetic moment and relatively strong exchange interactions of 3d transition metals (M) with the anisotropy naturally provided by lanthanide (Ln) ions is especially promising. Several molecular clusters of this type have been reported, such as {Mn 4 Ln 4 }, 10 {Mn 12 Gd}, 11 and {Cr 4 Dy 4 }, 12 with Ln = heavy Ln's, and {Mn 11 Ln 2 }, 13,14 with Ln = light rare earths. It was found that, in particular, Dy(III) ions are very useful for introducing anisotropy into these molecules, 15 thus confirming the possibility of achieving increased anisotropy in the lanthanide-transition-metal molecular combination.…”

Section: Introductionmentioning

confidence: 99%

Field-induced internal Fe and Ln spin reorientation in butterfly{Fe3LnO2}(Ln
Badía-Romano
¹
,
Bartolomé
²
,
Bartolomé
³

et al. 2013
Phys. Rev. B
21
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The intramolecular exchange interactions within the single-molecule magnet (SMM) "butterfly" molecule [Fe 3 Ln(μ 3 -O) 2 (CCl 3 COO) 8 (H 2 O)(THF) 3 ], where Ln(III) represents a lanthanide cation, are determined in a combined experimental [x-ray magnetic circular dichroism (XMCD) and vibrating sample magnetometer (VSM)] and theoretical work. Compounds with Ln = Gd and Dy, which represent extreme cases where the rare earth presents single-ion isotropic and uniaxial anisotropy, on one hand, and with Ln = Lu and Y(III) as pseudolanthanide substitutions that supply a nonmagnetic Ln reference case, on the other hand, are studied. The Dy single-ion uniaxial anisotropy is estimated from ab initio calculations. Low-temperature (T 2.5 K) hard x-ray XMCD at the Ln L 2,3 edges and VSM measurements as a function of the field indicate that the Ln moment dominates the polarization of the molecule by the applied field. Within the {Fe 3 LnO 2 } cluster the Ln-Fe 3 subcluster interaction is determined to be antiferromagnetic in both Dy and Gd compounds, with values J Dy-Fe 3 = −0.4 K and J Gd-Fe 3 = −0.25 K, by fitting to spin Hamiltonian simulations that consider the competing effects of intracluster interactions and the external applied magnetic field. In the uniaxial anisotropic {Fe 3 DyO 2 } case, a field-induced reorientation of the Fe 3 and Dy spins from an antiparallel to a parallel orientation takes place at a threshold field (μ 0 H = 4 T). In contrast, in isotropic {Fe 3 GdO 2 } this reorientation does not occur.

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“…[4][5][6][7][8] Initially, much work concentrated on mixing 4f ions with Mn III . However, experience shows that relatively isotropic ions can also be used to help aggregate 3d-4f clusters in such a way as to produce new examples of SMMs often with enhanced SMM properties compared with the pure 3d analogues.…”

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An Octanuclear [Cr^III₄Dy^III₄] 3d–4f Single‐Molecule Magnet

et al. 2010

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A Bell-Shaped Mn₁₁Gd₂ Single-Molecule Magnet

Cited by 292 publications

References 18 publications

High spin cycles: topping the spin record for a single molecule verging on quantum criticality

High spin cycles: topping the spin record for a single molecule verging on quantum criticality

Field-induced internal Fe and Ln spin reorientation in butterfly{Fe3LnO2}(Ln
Badía-Romano
¹
,
Bartolomé
²
,
Bartolomé
³

et al. 2013
Phys. Rev. B
21
2
14
0
View full text Add to dashboard Cite

An Octanuclear [Cr^III₄Dy^III₄] 3d–4f Single‐Molecule Magnet

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A Bell-Shaped Mn11Gd2 Single-Molecule Magnet

Cited by 292 publications

References 18 publications

High spin cycles: topping the spin record for a single molecule verging on quantum criticality

High spin cycles: topping the spin record for a single molecule verging on quantum criticality

Field-induced internal Fe and Ln spin reorientation in butterfly{Fe3LnO2}(LnBadía-Romano1, Bartolomé2, Bartolomé3 et al. 2013Phys. Rev. B212140View full textAdd to dashboardCite

An Octanuclear [CrIII4DyIII4] 3d–4f Single‐Molecule Magnet

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A Bell-Shaped Mn₁₁Gd₂ Single-Molecule Magnet

Field-induced internal Fe and Ln spin reorientation in butterfly{Fe3LnO2}(Ln
Badía-Romano
¹
,
Bartolomé
²
,
Bartolomé
³

et al. 2013
Phys. Rev. B
21
2
14
0
View full text Add to dashboard Cite

An Octanuclear [Cr^III₄Dy^III₄] 3d–4f Single‐Molecule Magnet