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The emergence of complex electronic behaviour from simple ingredients hasresulted in the discovery of numerous states of matter. Many examples are foundin systems exhibiting geometric magnetic frustration, which preventssimultaneous satisfaction of all magnetic interactions. This frustration givesrise to complex magnetic properties such as chiral spin structuresorbitally-driven magnetism, spin-ice behavior exhibiting Dirac strings withmagnetic monopoles, valence bond solids, and spin liquids. Here we report thesynthesis and characterization of LiZn2Mo3O8, a geometrically frustratedantiferromagnet in which the magnetic moments are localized on small transitionmetal clusters rather than individual ions. By doing so, first orderJahn-Teller instabilities and orbital ordering are prevented, allowing thestrongly interacting magnetic clusters in LiZn2Mo3O8 to probably give rise toan exotic condensed valence-bond ground state reminiscent of the proposedresonating valence bond state. Our results also link magnetism on clusters togeometric magnetic frustration in extended solids, demonstrating a new approachfor unparalleled chemical control and tunability in the search for collective,emergent electronic states of matter.

Possible valence-bond condensation in the frustrated cluster magnet LiZn2Mo3O8