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

References in corpus (7)

• Magnetic Order versus superconductivity in the Iron-based layered La(O1-xFx)FeAs systems
• Artificial "spin ice" in a geometrically frustrated lattice of nanoscale ferromagnetic islands
• Spin Dynamics of the Spin-1/2 Kagome Lattice Antiferromagnet ZnCu_3(OH)_6Cl_2
• Dirac Strings and Magnetic Monopoles in Spin Ice Dy2Ti2O7
• Spin-Liquid State in the S = 1/2 Hyperkagome Antiferromagnet Na4Ir3O8
• Spin chirality on a two-dimensional frustrated lattice
• Pinwheel VBS state and triplet excitations in the two-dimensional deformed kagome lattice

Cited by in corpus (20)

• Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO4
• Mixed-Valence-Driven Heavy-Fermion Behavior and Superconductivity in KNi${}_2$Se${}_2$
• Tunable Magnetic Transition to a Singlet Ground State in a 2D Van der Waals Layered Trimerized Kagomé Magnet
• Rearrangement of Van-der-Waals Stacking and Formation of a Singlet State at $T=90$ K in a Cluster Magnet
• 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
• Coulomb liquid phases of bosonic cluster Mott insulators on a pyrochlore lattice
• Unconventional magnetism in the spin-orbit driven Mott insulators Ba3MIr2O9 (M=Sc,Y)
• Emergence of string-valence bond solid state in the frustrated $J_1-J_2$ transverse field Ising model on the square lattice
• Quantum-critical scaling properties of the two-dimensional random-singlet state
• Electronic tunability of the frustrated triangular-lattice cluster magnet LiZn${}_{2-x}$Mo${}_3$O${}_8$
• 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
• Raman study of magnetic excitations and magneto-elastic coupling in alpha-SrCr2O4
• Band-Mott mixing hybridizes the gap in Fe${}_2$Mo${}_3$O${}_8$
• Robust atomic orbital in the cluster magnet LiMoO2
• Clusterization transition between cluster Mott insulators on a breathing Kagomé lattice
• Controlling the stoichiometry of the triangular lattice antiferromagnet Li${}_{1+x}$Zn${}_{2-y}$Mo${}_3$O${}_8$
• Classical Heisenberg and planar spin models on the windmill lattice
• Multipeak quasielastic light scattering and high-frequency electronic excitations in honeycomb Li${}_2$RuO${}_3$