Design of metal-complex magnets. Syntheses and magnetic properties of mixed-metal assemblies {NBu4[MCr(ox)3]}x (NBu4+ = tetra(n-butyl)ammonium ion; ox2- = oxalate ion; M = Mn2+, Fe2+, Co2+, Ni2+, Cu2+, Zn2+)

Tamaki, Hiroko; Zhong, Zhuang Jin; Matsumoto, Naohide; Kida, Sigeo; Koikawa, Masayuki; Achiwa, N.; Hashimoto, Y.; Ökawa, Hisashi

doi:10.1021/ja00044a004

Cited by 791 publications

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“…More interestingly, there are other 3D tricoordinated lattices with exotic Majorana states, which have not been found in iridates but are possible in 3D MOFs. Among these, the hyperoctagon lattice or (10,3)-a structure [36][37][38][39][40][41][42][43] has Majorana Fermi surfaces, which would be destabilized by an additional time-reversal interaction leaving an odd number of nodal lines [44,45].…”

Section: Fig 1 (Color Online) (A)mentioning

confidence: 99%

Designing Kitaev Spin Liquids in Metal-Organic Frameworks

2017

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Kitaev's honeycomb lattice spin model is a remarkable exactly solvable model, which has a particular type of spin liquid (Kitaev spin liquid) as the ground state. Although its possible realization in iridates and α-RuCl3 has been vigorously discussed recently, these materials have substantial non-Kitaev direct exchange interactions and do not have a spin liquid ground state. We propose metal-organic frameworks (MOFs) with Ru 3+ (or Os 3+ ) forming the honeycomb lattice as promising candidates for a more ideal realization of Kitaev-type spin models where the direct exchange interaction is strongly suppressed. The great flexibility of MOFs allows generalization to other three-dimensional lattices, for potential realization of a variety of spin liquids such as a Weyl spin liquid.PhySH: Frustrated magnetism, Spin liquid, Quantum spin liquid, Organic compoundsIntroduction. -Quantum spin liquids, purported exotic states of quantum magnets where long-range magnetic orders are destroyed by quantum fluctuations, have been a central subject in quantum magnetism [1]. As an important theoretical breakthrough, Kitaev constructed a spin-1/2 model on the honeycomb lattice [2] with Ising interactions between spin components depending on bond orientations. Its exact solution demonstrates many intriguing properties such as fractionalized anyonic excitations. This model was later generalized to other lattices, including three-dimensional ones, still retaining the exact solvability [3]. In this paper, we call this type of model including various generalizations as Kitaev model, and its ground states as Kitaev spin liquids. Jackeli and Khaliullin [4] discovered that the "Kitaev interaction", namely bond-dependent Ising couplings, can be realized in a (111) honeycomb layer of iridates, i.e. the A 2 IrO 3 (A = Na, Li) structure, by the superexchange interaction through the oxygen ions due to the strong spin-orbit coupling of Ir 4+ in the Mott insulator limit (see also Ref.[5] for the itinerant limit).However, unfortunately, it turned out that iridates and related inorganic compounds, such as α-RuCl 3 [6], exhibit a conventional magnetic order at low enough temperatures and do not have a true spin liquid ground state. This is due to the non-Kitaev interactions, such as antiferromagnetic Heisenberg interaction, mainly coming from the direct exchange interaction between the metal ions [7]. While their finite-temperature properties still reflect the proximity to the Kitaev model [8] and thus are of great interest, the current situation calls for a more ideal realization of the Kitaev model in real materials, so that they exhibit spin liquid ground states.In this Letter, we propose such a possible realization of the Kitaev model in metal-organic frameworks (MOFs), crystalline materials consisting of metal ions and bridging organic ligands. Although MOF is a central subject in modern complex chemistry, MOFs have not attracted much attention in the context of magnetism. This is

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Section: Fig 1 (Color Online) (A)mentioning

confidence: 99%

Designing Kitaev Spin Liquids in Metal-Organic Frameworks

2017

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“…The similarity of the Mössbauer spectra of (PPh 4 and M III are 3d ions, and ͑ox͒ is the oxalate anion, C 2 O 4 2Ϫ , are attractive systems in which to observe the establishment of magnetic correlations in two-dimensional honeycomb lattices, and as such they have been the subject of numerous studies. [1][2][3][4][5][6] In these insulating materials, the M II and M III cations are disposed in an alternating honeycomb array, bridged by oxalates so that each metal has a trigonally distorted octahedral environment, and the A cations lie in between the metal-oxalate layers, often with one or more side chains penetrating into the hexagonal cavities between the oxalates. Among the many compounds of this type, those containing Fe II and Fe III have proved particularly fascinating.…”

Section: Fementioning

confidence: 99%

Polarized neutron diffraction and Mössbauer spectral study of short-range magnetic correlations in the ferrimagnetic layered compounds(PPh4)[<

et al. 2002

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3 ͔ between 10 and 30 K of broad sextets and doublets in the Mössbauer spectra and the paramagnetic scattering observed in the polarized neutron measurements indicate the coexistence of spin-correlated and spin-uncorrelated regions in the layers of this compound. The polarized neutron scattering profiles and the Mössbauer spectra yield the magnetic exchange correlation length and lifetime, respectively, and the combined results are best understood in terms of layers composed of random frozen, but exchange correlated domains of ca. 50 Å diameter at the lowest temperatures, of spin-correlated domains and spin-uncorrelated regions at intermediate temperatures, and of largely spin-uncorrelated regions above the Néel temperature as determined from magnetometry. The similarity of the Mössbauer spectra of (PPh 4 ) ͓Fe II Fe III (ox) 3 ͔ and (NBu 4 ) ͓Fe II Fe III (ox) 3 ͔ leads to the conclusion that similar magnetic exchange correlations are present in the latter compound.

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“…Since their discovery [289], the rational design of oxalate-based bimetallic networks was followed by a sorting into two robust categories: (10,3) three-dimensional (3D) networks and (6,3) threedimensional (2D) networks [290]. Based on this rationalisation, it was possible to synthesize targeted multifunctional magnets to observe cross-e↵ects such as magneto-chiral dichroism [291] or magnetisation-induced second harmonic generation, for example [292].…”

Section: Introductionmentioning

confidence: 99%

From Mononuclear to Dinuclear: Magnetic Properties of Transition Metal Complexes

Saureu¹

2016

ioChem-BD Computational Chemistry Datasets

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Design of metal-complex magnets. Syntheses and magnetic properties of mixed-metal assemblies {NBu4[MCr(ox)3]}x (NBu4+ = tetra(n-butyl)ammonium ion; ox2- = oxalate ion; M = Mn2+, Fe2+, Co2+, Ni2+, Cu2+, Zn2+)

Cited by 791 publications

References 0 publications

Designing Kitaev Spin Liquids in Metal-Organic Frameworks

Designing Kitaev Spin Liquids in Metal-Organic Frameworks

Polarized neutron diffraction and Mössbauer spectral study of short-range magnetic correlations in the ferrimagnetic layered compounds(PPh4)[<

From Mononuclear to Dinuclear: Magnetic Properties of Transition Metal Complexes

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