Site-specific structure at multiple length scales in kagome quantum spin liquid candidates

Smaha, Rebecca W.; Boukahil, Idris; Titus, Charles J.; Jiang, Jack M.; Sheckelton, John P.; He, Wei; Wen, Jiajia; Vinson, John; Wang, SuYin Grass; Chen, Yu-Sheng; Teat, Simon J.; Devereaux, Thomas P.; Das Pemmaraju, C.; Lee, Young S.

doi:10.1103/PhysRevMaterials.4.124406

Title: Site-specific structure at multiple length scales in kagome quantum spin liquid candidates

Journal Article · Mon Dec 14 00:00:00 EST 2020 · Physical Review Materials

DOI:https://doi.org/10.1103/PhysRevMaterials.4.124406· OSTI ID:1762232

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SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
Stanford Univ., CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Realizing a quantum spin liquid (QSL) ground state in a real material is a leading issue in condensed matter physics research. In this pursuit, it is crucial to fully characterize the structure and influence of defects, as these can significantly affect the fragile QSL physics. In this work, we perform a variety of cutting-edge synchrotron x-ray scattering and spectroscopy techniques, and we advance new methodologies for site-specific diffraction and L-edge Zn absorption spectroscopy. The experimental results along with our first-principles calculations address outstanding questions about the local and long-range structures of the two leading kagome QSL candidates, Zn-substituted barlowite Cu₃Zn_xCu_1-x(OH)₆FBr and herbertsmithite Cu₃Zn(OH)₆Cl₂. On all length scales probed, there is no evidence that Zn substitutes onto the kagome layers, thereby preserving the QSL physics of the kagome lattice. Our calculations show that antisite disorder is not energetically favorable and is even less favorable in Zn-barlowite compared to herbertsmithite. Site-specific x-ray diffraction measurements of Zn-barlowite reveal that Cu²⁺ and Zn²⁺ selectively occupy distinct interlayer sites, in contrast to herbertsmithite. Using the first measured Zn L-edge inelastic x-ray absorption spectra combined with calculations, we discover a systematic correlation between the loss of inversion symmetry from pseudo-octahedral (herbertsmithite) to trigonal prismatic coordination (Zn-barlowite) with the emergence of a new peak. Overall, our measurements suggest that Zn-barlowite has structural advantages over herbertsmithite that make its magnetic properties closer to an ideal QSL candidate: its kagome layers are highly resistant to nonmagnetic defects while the interlayers can accommodate a higher amount of Zn substitution.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS) and National Energy Research Scientific Computing Center (NERSC); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Stanford Univ., CA (United States)

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

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; AC02-06CH11357; NSF/CHE-1834750; ECCS-2026822

OSTI ID:: 1762232

Alternate ID(s):: OSTI ID: 1755517; OSTI ID: 1779169

Journal Information:: Physical Review Materials, Vol. 4, Issue 12; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
Quantum spin liquid
Kagome lattice
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First-principles calculations
Resonant elastic x-ray scattering
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X-ray absorption spectroscopy
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CSD 1995564: Experimental Crystal Structure Determination W., Smaha, Rebecca; Idris, Boukahil,; J., Titus, Charles https://doi.org/10.25505/fiz.icsd.cc24zk1r The current record is supplemented by this dataset	dataset	January 2020
CSD 1899248: Experimental Crystal Structure Determination W., Smaha, Rebecca; Idris, Boukahil,; J., Titus, Charles https://doi.org/10.25505/fiz.icsd.cc21rb27 The current record is supplemented by this dataset	dataset	January 2020
CSD 1899246: Experimental Crystal Structure Determination W., Smaha, Rebecca; Idris, Boukahil,; J., Titus, Charles https://doi.org/10.25505/fiz.icsd.cc21rb05 The current record is supplemented by this dataset	dataset	January 2020

Title: Site-specific structure at multiple length scales in kagome quantum spin liquid candidates

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