Tunable Quantum Spin Liquidity in the 
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th-Filled Breathing Kagome Lattice

Akbari-Sharbaf, Arash; Sinclair, R.; Verrier, A.; Ziat, Djamel; Zhou, H. D.; Sun, Xiaofeng; Quilliam, J. A.

doi:10.1103/physrevlett.120.227201

Cited by 30 publications

(25 citation statements)

References 39 publications

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“…Our first-principles calculations would possibly rule out some previous scenarios proposed within the same model for decoupling 2/3 of the spins in LiZn 2 Mo 3 O 8 at low temperatures, such as a U(1) QSL state with the spinon Fermi surface 22 and strong coupling between next-nearest neighbours 34,37 . Cooperative rotations of the Mo 3 O 13 clusters resulting in an emergent hexagonal lattice 21 assume electrons to be well localised at the clusters and are at variance with our results in the strong interaction limit.…”

Section: Discussionsupporting

confidence: 53%

Quantum spin liquid and cluster Mott insulator phases in the Mo3O8 magnets

2021

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We unveil the microscopic origin of largely debated magnetism in the Mo3O8 quantum systems. Upon considering an extended Hubbard model at 1/6 filling on the anisotropic kagomé lattice formed by the Mo atoms, we argue that its ground state is determined by the competition between kinetic energy and intersite Coulomb interactions, which is controlled by the trimerisation of the kagomé lattice into the Mo3O13 clusters, and the sign of hopping parameters, specifying the electron localisation at such clusters. Based on first-principles calculations, we show that the strong interaction limit reveals a plaquette charge order with unpaired spins at the resonating hexagons that can be realised in LiZn2Mo3O8, and whose origin is solely related to the opposite signs of intracluster and intercluster hoppings, in contrast to all previous scenarios. On the other hand, both Li2InMo3O8 and Li2ScMo3O8 are demonstrated to fall into the weak interaction limit where the electrons are well localised at the Mo3O13 clusters. While the former is found to exhibit long-range antiferromagnetic order, the latter is more likely to reveal short-range order with quantum spin liquid-like excitations. Our results not only reproduce most of the experimentally observed features of the Mo3O8 systems, but will also help to describe various properties in other quantum cluster magnets.

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Section: Discussionsupporting

confidence: 53%

Quantum spin liquid and cluster Mott insulator phases in the Mo3O8 magnets

2021

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“…This may be detected by high-resolution Xray scattering or X-ray pair distribution function (PDF) measurement. The plaquette charge order reconstructs the spin states within each resonant hexagon leading to the freezing of 2/3 of the spins, as observed in the spin susceptibility in LiZn 2 Mo 3 O 8 [21][22][23][24][25] . A different explanation of the susceptibility anomaly in LiZn 2 Mo 3 O 8 based on the lattice distortion and the emergent lattices has been proposed in a previous work 26 .…”

Section: Discussionmentioning

confidence: 86%

“…Such a charge-driven spin-state-reconstruction is one crucial property of the CMI in this system 6 8 20 , where the Mo electrons are in the CMI with the Mo electrons localized in the smaller triangular clusters of the distorted Kagome lattice (see Fig. 1) [21][22][23][24][25] . The distortion is such that the up and down triangles have different bond lengths and the lattice is often referred to as the breathing kagome.…”

Section: Introductionmentioning

confidence: 94%

Emergent orbitals in the cluster Mott insulator on a breathing kagome lattice

Chen

Lee

2018

Phys. Rev. B

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Motivated by the recent developments on cluster Mott insulating materials such as the cluster magnet LiZn2Mo3O8, we consider the strong plaquette charge ordered regime of the extended Hubbard model on a breathing Kagome lattice and reveal the properties of the cluster Mottness. The plaquette charge order arises from the inter-site charge interaction and the collective motion of three localized electrons on the hexagon plaquettes. This model leads naturally to a reduction of the local moments by 2/3 as observed in LiZn2Mo3O8. Furthermore, at low temperatures each hexagon plaquette contains an extra orbital-like degree of freedom in addition to the remaining spin 1/2. We explore the consequence of this emergent orbital degree of freedom. We point out the interaction between the local moments is naturally described by a Kugel-Khomskii spin-orbital model. We develop a parton approach and suggest a spin liquid ground state with spinon Fermi surfaces for this model. We further predict an emergent orbital order when the system is under a strong magnetic field. Various experimental consequences for LiZn2Mo3O8 are discussed, including an argument that the charge ordering much be short ranged if the charge per Mo is slightly off stoichiometry.

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“…In fact, the gap-like excitation was observed in the long-range ordered state of Ba 3 CoSb 2 O 9 13,14 , whereas the gapless magnetic excitations in the QSL systems YbMgGaO 4 21,22 and Ba 3 NiSb 2 O 9 26 . INS measurements on magnetic excitations in the substitution system Li 2 (In 1− x Sc x )Mo 3 O 8 40 are effective to further elucidate the origin of different magnetic ground states, which is left for future work.…”

Section: Resultsmentioning

confidence: 99%

Quantum magnetisms in uniform triangular lattices Li2AMo3O8 (A = In, Sc)

Iida

Yoshida

Okabe

et al. 2019

Sci Rep

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Molecular based spin-1/2 triangular lattice systems such as LiZn2Mo3O8 have attracted research interest. Distortions, defects, and intersite disorder are suppressed in such molecular-based magnets, and intrinsic geometrical frustration gives rise to unconventional and unexpected ground states. Li2AMo3O8 (A = In or Sc) is such a compound where spin-1/2 Mo3O13 clusters in place of Mo ions form the uniform triangular lattice. Their ground states are different according to the A site. Li2InMo3O8 undergoes conventional 120° long-range magnetic order below TN = 12 K whereas isomorphic Li2ScMo3O8 exhibits no long-range magnetic order down to 0.5 K. Here, we report exotic magnetisms in Li2InMo3O8 and Li2ScMo3O8 investigated by muon spin rotation (μSR) and inelastic neutron scattering (INS) spectroscopies using polycrystalline samples. Li2InMo3O8 and Li2ScMo3O8 show completely different behaviors observed in both μSR and INS measurements, representing their different ground states. Li2InMo3O8 exhibits spin wave excitation which is quantitatively described by the nearest neighbor anisotropic Heisenberg model based on the 120° spin structure. In contrast, Li2ScMo3O8 undergoes short-range magnetic order below 4 K with quantum-spin-liquid-like magnetic fluctuations down to the base temperature. Origin of the different ground states is discussed in terms of anisotropies of crystal structures and magnetic interactions.

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Tunable Quantum Spin Liquidity in the 1/6 th-Filled Breathing Kagome Lattice

Cited by 30 publications

References 39 publications

Quantum spin liquid and cluster Mott insulator phases in the Mo3O8 magnets

Quantum spin liquid and cluster Mott insulator phases in the Mo3O8 magnets

Emergent orbitals in the cluster Mott insulator on a breathing kagome lattice

Quantum magnetisms in uniform triangular lattices Li2AMo3O8 (A = In, Sc)

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