Emergence of spin singlets with inhomogeneous gaps in the kagome lattice Heisenberg antiferromagnets Zn-barlowite and herbertsmithite

Wang, Jiaming; Yuan, Weishi; Singer, Philip M.; Smaha, Rebecca W.; He, Wei; Wen, Jiajia; Lee, Young S.; Imai, Takashi

doi:10.1038/s41567-021-01310-3

Title: Emergence of spin singlets with inhomogeneous gaps in the kagome lattice Heisenberg antiferromagnets Zn-barlowite and herbertsmithite

Journal Article · Thu Aug 05 00:00:00 EDT 2021 · Nature Physics

DOI:https://doi.org/10.1038/s41567-021-01310-3· OSTI ID:1819280

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McMaster Univ., Hamilton, ON (Canada)
Rice Univ., Houston, TX (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); Stanford Univ., CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)

The kagome Heisenberg antiferromagnet formed by frustrated spins arranged in a lattice of corner-sharing triangles is a prime candidate for hosting a quantum spin liquid (QSL) ground state consisting of entangled spin singlets. However, the existence of various competing states makes a convincing theoretical prediction of the QSL ground state difficult, calling for experimental clues from model materials. The kagome lattice materials Zn-barlowite (ZnCu₃(OD)₆FBr) and herbertsmithite (ZnCu₃(OD)₆Cl₂) do not exhibit long-range order and are considered the best realizations of the kagome Heisenberg antiferromagnet known so far. In this study, we use ⁶³Cu nuclear quadrupole resonance combined with the inverse Laplace transform to locally probe the inhomogeneity of delicate quantum ground states affected by disorder. We present direct evidence for the gradual emergence of spin singlets with spatially varying excitation gaps, but even at temperatures far below the super-exchange energy scale their fraction is limited to ~60% of the total spins. Theoretical models need to incorporate the role of disorder to account for the observed inhomogeneously gapped behaviour.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

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

Grant/Contract Number:: AC02-76SF00515; DGE-1656518

OSTI ID:: 1819280

Journal Information:: Nature Physics, Vol. 17; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

References (33)

Spin liquids in frustrated magnets Balents, Leon Nature, Vol. 464, Issue 7286 https://doi.org/10.1038/nature08917	journal	March 2010
Gapped Spin-1/2 Spinon Excitations in a New Kagome Quantum Spin Liquid Compound Cu ₃ Zn(OH) ₆ FBr Feng, Zili; Li, Zheng; Meng, Xin Chinese Physics Letters, Vol. 34, Issue 7 https://doi.org/10.1088/0256-307X/34/7/077502	journal	June 2017
Valence Bond Glass Phase in Dilute Kagome Antiferromagnets Singh, R. R. P. Physical Review Letters, Vol. 104, Issue 17 https://doi.org/10.1103/PhysRevLett.104.177203	journal	April 2010
Spin-1/2 Kagomé -Like Lattice in Volborthite Cu ₃ V ₂ O ₇ (OH) ₂ ·2H ₂ O Hiroi, Zenji; Hanawa, Masafumi; Kobayashi, Naoya Journal of the Physical Society of Japan, Vol. 70, Issue 11 https://doi.org/10.1143/JPSJ.70.3377	journal	November 2001
Exact Dimer Ground State and Quantized Magnetization Plateaus in the Two-Dimensional Spin System ${SrCu}_{2} ({BO}_{3})_{2}$ Kageyama, H.; Yoshimura, K.; Stern, R. Physical Review Letters, Vol. 82, Issue 15 https://doi.org/10.1103/PhysRevLett.82.3168	journal	April 1999
Quantum spin liquids Broholm, C.; Cava, R. J.; Kivelson, S. A. Science, Vol. 367, Issue 6475 https://doi.org/10.1126/science.aay0668	journal	January 2020
Projected-Wave-Function Study of the Spin- $1 / 2$ Heisenberg Model on the Kagomé Lattice Ran, Ying; Hermele, Michael; Lee, Patrick A. Physical Review Letters, Vol. 98, Issue 11 https://doi.org/10.1103/PhysRevLett.98.117205	journal	March 2007
Spin-Liquid Ground State of the S = 1/2 Kagome Heisenberg Antiferromagnet Yan, S.; Huse, D. A.; White, S. R. Science, Vol. 332, Issue 6034 https://doi.org/10.1126/science.1201080	journal	April 2011
T1–T2 Correlation Spectra Obtained Using a Fast Two-Dimensional Laplace Inversion Song, Y. -Q.; Venkataramanan, L.; Hürlimann, M. D. Journal of Magnetic Resonance, Vol. 154, Issue 2 https://doi.org/10.1006/jmre.2001.2474	journal	February 2002
Magnetic resonance as a local probe for kagomé magnetism in Barlowite Cu4(OH)6FBr Ranjith, K. M.; Klein, C.; Tsirlin, A. A. Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-29080-8	journal	July 2018
Resolving Dirac electrons with broadband high-resolution NMR Papawassiliou, Wassilios; Jaworski, Aleksander; Pell, Andrew J. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-14838-4	journal	March 2020
Nuclear Magnetic Relaxation in Antiferromagnetics, II Moriya, Tôru Progress of Theoretical Physics, Vol. 16, Issue 6 https://doi.org/10.1143/PTP.16.641	journal	December 1956
${}^{139}{La}$ NMR investigation of the interplay between lattice, charge, and spin dynamics in the charge-ordered high- $T_{c}$ cuprate ${La}_{1.875} {Ba}_{0.125} {CuO}_{4}$ Singer, P. M.; Arsenault, A.; Imai, T. Physical Review B, Vol. 101, Issue 17 https://doi.org/10.1103/PhysRevB.101.174508	journal	May 2020
A Structurally Perfect S = ¹ / ₂ Kagomé Antiferromagnet Shores, Matthew P.; Nytko, Emily A.; Bartlett, Bart M. Journal of the American Chemical Society, Vol. 127, Issue 39 https://doi.org/10.1021/ja053891p	journal	October 2005
Dynamic Scaling in the Susceptibility of the Spin- $\frac{1}{2}$ Kagome Lattice Antiferromagnet Herbertsmithite Helton, J. S.; Matan, K.; Shores, M. P. Physical Review Letters, Vol. 104, Issue 14 https://doi.org/10.1103/PhysRevLett.104.147201	journal	April 2010
Local spin susceptibility of the $S = \frac{1}{2}$ kagome lattice in ZnCu $_{3}$ (OD) $_{6}$ Cl $_{2}$ Imai, T.; Fu, M.; Han, T. H. Physical Review B, Vol. 84, Issue 2 https://doi.org/10.1103/PhysRevB.84.020411	journal	July 2011
Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet Han, Tian-Heng; Helton, Joel S.; Chu, Shaoyan Nature, Vol. 492, Issue 7429 https://doi.org/10.1038/nature11659	journal	December 2012
Scaling and data collapse from local moments in frustrated disordered quantum spin systems Kimchi, Itamar; Sheckelton, John P.; McQueen, Tyrel M. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-06800-2	journal	October 2018
Site-specific structure at multiple length scales in kagome quantum spin liquid candidates Smaha, Rebecca W.; Boukahil, Idris; Titus, Charles J. Physical Review Materials, Vol. 4, Issue 12 https://doi.org/10.1103/PhysRevMaterials.4.124406	journal	December 2020
Nuclear Quadrupole Resonance of Cu in the Paramagnetic State of CuO Itoh, Yutaka; Imai, Takashi; Shimizu, Tadashi Journal of the Physical Society of Japan, Vol. 59, Issue 4 https://doi.org/10.1143/JPSJ.59.1143	journal	April 1990
Evidence for a gapped spin-liquid ground state in a kagome Heisenberg antiferromagnet Fu, M.; Imai, T.; Han, T. -H. Science, Vol. 350, Issue 6261 https://doi.org/10.1126/science.aab2120	journal	November 2015
${}^{63}{Cu}$ , ${}^{35}{Cl}$ , and ${}^{1}H$ NMR in the $S = \frac{1}{2}$ Kagome Lattice ${ZnCu}_{3} (OH)_{6} {Cl}_{2}$ Imai, T.; Nytko, E. A.; Bartlett, B. M. Physical Review Letters, Vol. 100, Issue 7 https://doi.org/10.1103/PhysRevLett.100.077203	journal	February 2008
Gapless Spin-Liquid Ground State in the $S = 1 / 2$ Kagome Antiferromagnet Liao, H. J.; Xie, Z. Y.; Chen, J. Physical Review Letters, Vol. 118, Issue 13 https://doi.org/10.1103/PhysRevLett.118.137202	journal	March 2017
Cu Nuclear Quadrupole Resonance Study of CuGeO ₃ Kikuchi, Jun; Yasuoka, Hiroshi; Hase, Masashi Journal of the Physical Society of Japan, Vol. 63, Issue 3 https://doi.org/10.1143/JPSJ.63.872	journal	March 1994
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 npj Quantum Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s41535-020-0222-8	journal	April 2020
Observation of a Spin Gap in Sr ${Cu}_{2}$ $O_{3}$ Comprising Spin-½ Quasi-1D Two-Leg Ladders Azuma, M.; Hiroi, Z.; Takano, M. Physical Review Letters, Vol. 73, Issue 25 https://doi.org/10.1103/PhysRevLett.73.3463	journal	December 1994
Pinwheel valence-bond solid and triplet excitations in the two-dimensional deformed kagome lattice Matan, K.; Ono, T.; Fukumoto, Y. Nature Physics, Vol. 6, Issue 11 https://doi.org/10.1038/nphys1761	journal	September 2010
Site Specific X-ray Anomalous Dispersion of the Geometrically Frustrated Kagomé Magnet, Herbertsmithite, ZnCu ₃ (OH) ₆ Cl ₂ Freedman, Danna E.; Han, Tianheng H.; Prodi, Andrea Journal of the American Chemical Society, Vol. 132, Issue 45 https://doi.org/10.1021/ja1070398	journal	November 2010
A high-temperature quantum spin liquid with polaron spins Klanjšek, Martin; Zorko, Andrej; Žitko, Rok Nature Physics, Vol. 13, Issue 11 https://doi.org/10.1038/nphys4212	journal	July 2017
Spin Dynamics of the Spin- $1 / 2$ Kagome Lattice Antiferromagnet ${ZnCu}_{3} (OH)_{6} {Cl}_{2}$ Helton, J. S.; Matan, K.; Shores, M. P. Physical Review Letters, Vol. 98, Issue 10 https://doi.org/10.1103/PhysRevLett.98.107204	journal	March 2007
Symmetry Reduction in the Quantum Kagome Antiferromagnet Herbertsmithite Zorko, A.; Herak, M.; Gomilšek, M. Physical Review Letters, Vol. 118, Issue 1 https://doi.org/10.1103/PhysRevLett.118.017202	journal	January 2017
Gapless ground state in the archetypal quantum kagome antiferromagnet ZnCu3(OH)6Cl2 Khuntia, P.; Velazquez, M.; Barthélemy, Q. Nature Physics, Vol. 16, Issue 4 https://doi.org/10.1038/s41567-020-0792-1	journal	February 2020
Scaling Studies of Highly Disordered Spin-½ Antiferromagnetic Systems Bhatt, R. N.; Lee, P. A. Physical Review Letters, Vol. 48, Issue 5 https://doi.org/10.1103/PhysRevLett.48.344	journal	February 1982

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