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.

arXiv comment30 pages, 10 figures

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• The Chemistry of Quantum Spin Liquids
• Scaling and data collapse from local moments in frustrated disordered quantum spin systems
• Structural instability of the rutile compounds and its relevance to the metal-insulator transition of VO2
• Hexagonal Perovskites as Quantum Materials
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• Mixed-Valence-Driven Heavy-Fermion Behavior and Superconductivity in KNi${}_2$Se${}_2$
• Molecular Quantum Magnetism in LiZn2Mo3O8
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• Survival of itinerant excitations and quantum spin state transitions in YbMgGaO${}_4$ with chemical disorder
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• Emergent honeycomb lattice in LiZn2Mo3O8
• Cluster Mott insulators and two Curie-Weiss regimes on an anisotropic Kagome lattice
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• Emergent orbitals in the cluster Mott insulator on a breathing Kagome lattice
• Tunable quantum spin liquidity in the 1/6th-filled breathing kagome lattice
• Multiflavor Mott insulators in quantum materials and ultracold atoms
• Microscopic toy model for magnetoelectric effect in polar Fe${}_2$Mo${}_3$O${}_8$
• The trimer-based spin liquid candidate Ba4NbIr3O12
• Quantum spin liquid and cluster Mott insulator phases in the Mo${}_3$O${}_8$ magnets
• Fractionalized charge excitations in a spin liquid on partially-filled pyrochlore lattice
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• Unconventional magnetism in the spin-orbit driven Mott insulators Ba3MIr2O9 (M=Sc,Y)
• Cluster magnetism of Ba4NbMn3O12: localized electrons or molecular orbitals?
• LiZn${}_2$V${}_3$O${}_8$: A new geometrically frustrated cluster spin-glass
• Spin-orbit coupling and strong electronic correlations in cyclic molecules
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• Realization of the orbital-selective Mott state at the molecular level in Ba${}_3$LaRu${}_2$O${}_9$
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• Electronic tunability of the frustrated triangular-lattice cluster magnet LiZn${}_{2-x}$Mo${}_3$O${}_8$
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• Quantum magnetisms in uniform triangular lattices Li2AMo3O8 (A = In, Sc)
• Orbital Peierls mechanism of the formation of molecular clusters in Na2Ti3Cl8 and in similar systems
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• Raman study of magnetic excitations and magneto-elastic coupling in alpha-SrCr2O4
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• Quasimolecular $J_{\mathrm{tet}}$=3/2 moments in the cluster Mott insulator GaTa${}_4$Se${}_8$
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• Magnetoelectric behavior of breathing kagomé monolayers of ${\mathrm{Nb}}_3{(\mathrm{Cl},\mathrm{Br},\mathrm{I})}_8$ from first-principles calculations
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• Effects of anisotropy in spin molecular-orbital coupling on effective spin models of trinuclear organometallic complexes
• Controlling the stoichiometry of the triangular lattice antiferromagnet Li${}_{1+x}$Zn${}_{2-y}$Mo${}_3$O${}_8$
• Novel quantum spin liquid ground state in the trimer rhodate Ba${}_4$NbRh${}_3$O${}_{12}$
• Gapless dynamic magnetic ground state in the charge-gapped trimer iridate Ba${}_4$NbIr${}_3$O${}_{12}$
• Classical phase diagram of the stuffed honeycomb lattice
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• Multipeak quasielastic light scattering and high-frequency electronic excitations in honeycomb Li${}_2$RuO${}_3$
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• 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