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Possible valence-bond condensation in the frustrated cluster magnet LiZn2Mo3O8

Nature Materials volume 11, pages 493–496 (2012)Cite this article

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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 structures1,2,3, orbitally driven magnetism4, spin-ice behaviour5 exhibiting Dirac strings with magnetic monopoles6, valence-bond solids7,8 and spin liquids9,10. 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 ions11,12,13. 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 state14,15. 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 statesof matter16,17.

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Figure 1: LiZn2Mo3O8 structure.
Figure 2: Physical properties of LiZn2Mo3O8.

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Acknowledgements

This research is supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award DE-FG02-08ER46544. Use of the Spallation Neutron Source was supported by the Division of Scientific User Facilities, Office of Basic Energy Sciences, US Department of Energy, under contract DE-AC05-00OR22725 with UT-Battelle, LLC. J.P.S. acknowledges the assistance of J. Hodges in collecting and analysing powder neutron data from POWGEN/SNS. T.M.M. acknowledges useful discussions with O. Tchernyshyov and C. Broholm.

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Authors and Affiliations

  1. Department of Chemistry, Department of Physics and Astronomy, and the Institute for Quantum Matter, The Johns Hopkins University, Baltimore, Maryland 21218, USA

    J. P. Sheckelton, J. R. Neilson, D. G. Soltan & T. M. McQueen

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  1. J. P. Sheckelton
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  2. J. R. Neilson
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  3. D. G. Soltan
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Contributions

T.M.M. supervised the project. J.P.S. and D.G.S. prepared samples. J.P.S. measured neutron diffraction patterns. J.P.S. and T.M.M. measured properties, and J.P.S., J.R.N. and T.M.M. analysed data and prepared the manuscript.

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Correspondence to T. M. McQueen.

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Sheckelton, J., Neilson, J., Soltan, D. et al. Possible valence-bond condensation in the frustrated cluster magnet LiZn2Mo3O8. Nature Mater 11, 493–496 (2012). https://doi.org/10.1038/nmat3329

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