Materializing rival ground states in the barlowite family of kagome magnets: quantum spin liquid, spin ordered, and valence bond crystal states

Smaha, Rebecca W.; He, Wei; Jiang, Jack Mingde; Wen, Jiajia; Jiang, Yi-Fan; Sheckelton, John P.; Titus, Charles J.; Wang, Suyin Grass; Chen, Yu-Sheng; Teat, Simon J.; Aczel, Adam A.; Zhao, Yang; Xu, Guangyong; Lynn, Jeffrey W.; Jiang, Hong-Chen; Lee, Young S.

doi:10.1038/s41535-020-0222-8

Title: Materializing rival ground states in the barlowite family of kagome magnets: quantum spin liquid, spin ordered, and valence bond crystal states

Journal Article · Tue Apr 14 00:00:00 EDT 2020 · npj Quantum Materials

DOI:https://doi.org/10.1038/s41535-020-0222-8· OSTI ID:1617810

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SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., CA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Univ. of Chicago, IL (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)

The spin- $\frac{1}{2}$ kagome antiferromagnet is considered an ideal host for a quantum spin liquid ground state. We find that when the bonds of the kagome lattice are modulated with a periodic pattern, new quantum ground states emerge. Newly synthesized crystalline barlowite (Cu₄(OH)₆FBr) and Zn-substituted barlowite demonstrate the delicate interplay between singlet states and spin order on the spin- $\frac{1}{2}$ kagome lattice. Comprehensive structural measurements demonstrate that our new variant of barlowite maintains hexagonal symmetry at low temperatures with an arrangement of distorted and undistorted kagome triangles, for which numerical simulations predict a pinwheel va- lence bond crystal (VBC) state instead of a quantum spin liquid (QSL). The presence of interlayer spins eventually leads to an interesting pinwheel q=0 magnetic order. Partially Zn-substituted bar- lowite (Cu_3.44Zn_0.56(OH)₆FBr) has an ideal kagome lattice and shows QSL behavior, indicating a surprising robustness of the QSL against interlayer impurities. The magnetic susceptibility is simi- lar to that of herbertsmithite, even though the Cu²⁺ impurities are above the percolation threshold for the interlayer lattice and they couple more strongly to the nearest kagome moment. This system is a unique playground displaying QSL, VBC, and spin order, furthering our understanding of these highly competitive quantum states.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC02-76SF00515; AC02-05CH11231; AC02-06CH11357; CHE-1834750; DMR-1531283; ECCS-1542152; DGE-1656518

OSTI ID:: 1617810

Alternate ID(s):: OSTI ID: 1602253

Journal Information:: npj Quantum Materials, Vol. 5, Issue 1; ISSN 2397-4648

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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CSD 1899252: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21rb6c The current record is supplemented by this dataset	dataset	January 2020
CSD 1899243: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21r9x1 The current record is supplemented by this dataset	dataset	January 2020
CSD 1898753: Experimental Crystal Structure Determination W., Smaha, Rebecca; Wei, He,; Mingde, Jiang, Jack https://doi.org/10.25505/fiz.icsd.cc21qt3q The current record is supplemented by this dataset	dataset	January 2020
CSD 1899367: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21rfx5 The current record is supplemented by this dataset	dataset	January 2020
CSD 1899370: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21rg09 The current record is supplemented by this dataset	dataset	January 2020
CSD 1899242: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21r9w0 The current record is supplemented by this dataset	dataset	January 2020
CSD 1898752: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21qt2p The current record is supplemented by this dataset	dataset	January 2020
CSD 1898756: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21qt6t The current record is supplemented by this dataset	dataset	January 2020
CSD 1922923: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc22jysc The current record is supplemented by this dataset	dataset	January 2020
CSD 1898751: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21qt1n The current record is supplemented by this dataset	dataset	January 2020
CSD 1899250: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21rb49 The current record is supplemented by this dataset	dataset	January 2020
CSD 1899365: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21rfv3 The current record is supplemented by this dataset	dataset	January 2020
CSD 1899369: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21rfz7 The current record is supplemented by this dataset	dataset	January 2020
CSD 1898754: Experimental Crystal Structure Determination W., Smaha, R.; W., He,; M., Jiang, J. https://doi.org/10.25505/fiz.icsd.cc21qt4r The current record is supplemented by this dataset	dataset	January 2020

Title: Materializing rival ground states in the barlowite family of kagome magnets: quantum spin liquid, spin ordered, and valence bond crystal states

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