Possible valence-bond condensation in the frustrated cluster magnet LiZn2Mo3O8

Abstract

The emergence of complex electronic behaviour from simple ingredients has resulted in the discovery of numerous states of matter. Many examples are found in systems exhibiting geometric magnetic frustration, which prevents simultaneous satisfaction of all magnetic interactions. This frustration gives rise to complex magnetic properties such as chiral spin structures orbitally-driven magnetism, spin-ice behavior exhibiting Dirac strings with magnetic monopoles, valence bond solids, and spin liquids. Here we report the synthesis and characterization of LiZn2Mo3O8, a geometrically frustrated antiferromagnet in which the magnetic moments are localized on small transition metal clusters rather than individual ions. By doing so, first order Jahn-Teller instabilities and orbital ordering are prevented, allowing the strongly interacting magnetic clusters in LiZn2Mo3O8 to probably give rise to an exotic condensed valence-bond ground state reminiscent of the proposed resonating valence bond state. Our results also link magnetism on clusters to geometric magnetic frustration in extended solids, demonstrating a new approach for unparalleled chemical control and tunability in the search for collective, emergent electronic states of matter.

30 pages, 10 figures

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• Survival of itinerant excitations and quantum spin state transitions in YbMgGaO${}_4$ with chemical disorder
• Emergent orbitals in the cluster Mott insulator on a breathing Kagome lattice
• Multiflavor Mott insulators in quantum materials and ultracold atoms
• Quantum spin liquid and cluster Mott insulator phases in the Mo${}_3$O${}_8$ magnets
• Coulomb liquid phases of bosonic cluster Mott insulators on a pyrochlore lattice
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• Emergence of string-valence bond solid state in the frustrated $J_1-J_2$ transverse field Ising model on the square lattice
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• Quantum-critical scaling properties of the two-dimensional random-singlet state
• Magnetic molecular orbitals in MnSi
• Electronic tunability of the frustrated triangular-lattice cluster magnet LiZn${}_{2-x}$Mo${}_3$O${}_8$
• Orbital Peierls mechanism of the formation of molecular clusters in Na2Ti3Cl8 and in similar systems
• Quantum magnetisms in uniform triangular lattices Li2AMo3O8 (A = In, Sc)
• CrRhAs: a member of a large family of metallic kagome antiferromagnets
• Quasimolecular $J_{\mathrm{tet}}$=3/2 moments in the cluster Mott insulator GaTa${}_4$Se${}_8$
• Band-Mott mixing hybridizes the gap in Fe${}_2$Mo${}_3$O${}_8$
• Raman study of magnetic excitations and magneto-elastic coupling in alpha-SrCr2O4
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• Robust atomic orbital in the cluster magnet LiMoO2
• Quantum tricriticality of incommensurate phase induced by quantum domain walls in frustrated Ising magnetism
• Electronic Density of States of a $U\left(1\right)$ Quantum Spin Liquid with Spinon Fermi Surface. II. Zeeman Magnetic Field Effects
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• Controlling the stoichiometry of the triangular lattice antiferromagnet Li${}_{1+x}$Zn${}_{2-y}$Mo${}_3$O${}_8$
• Clusterization transition between cluster Mott insulators on a breathing Kagomé lattice
• Gapless dynamic magnetic ground state in the charge-gapped trimer iridate Ba${}_4$NbIr${}_3$O${}_{12}$
• Novel quantum spin liquid ground state in the trimer rhodate Ba${}_4$NbRh${}_3$O${}_{12}$
• Molecular Orbital Electronic Instability in the van der Waals Kagome Semiconductor Nb${}_3$Cl${}_8$: Exploring Future Directions
• Multipeak quasielastic light scattering and high-frequency electronic excitations in honeycomb Li${}_2$RuO${}_3$
• Classical Heisenberg and planar spin models on the windmill lattice
• Widely Spaced Planes of Magnetic Dimers in the Ba6Y2Rh2Ti2O17-δ Hexagonal Perovskite
• Partial magnetic order in kagome spin ice
• Doping effects on the valence bond solid of Li${}_2$RuO${}_3$ with Mn substitution
• Antiferromagnetic Spin Fluctuations and Structural Transition in Cluster Mott Insulator Candidate Nb3Cl8 Revealed by 93Nb- and 35Cl-NMR
• Valence-Bond Solid phases in the spin-$1/2$ Kekule-Heisenberg model
• Impact of Oxidation State on the Valence-bond-glass Physics in the lithium-intercalated Mo${}_3$O${}_8$ Cluster Mott Insulators
• Quasimolecular electronic structure of the trimer iridate Ba${}_4$NbIr${}_3$O${}_{12}$
• Stabilizing Itinerant Electrons in a Corner-Sharing Kagomé Oxide Nd4Os3ZnO14
• Magnetic ordering of the Mo${}_3$O${}_8$-type cluster Mott insulator Na${}_3$Sc${}_2$(MoO${}_4$)${}_2$Mo${}_3$O${}_8$ with spin-1/2 triangular lattice prepared via optimal synthesis
• Signatures of a Majorana-Fermi surface in the Kitaev magnet Ag${}_3$LiIr${}_2$O${}_6$
• Novel Quantum Spin Liquid States in the $S=\frac{1}{2}$ Three-Dimensional Compound Y${}_3$Cu${}_2$Sb${}_3$O${}_{14}$