Correlated impurities and intrinsic spin-liquid physics in the kagome material herbertsmithite
Abstract
Low energy inelastic neutron scattering on single crystals of the kagome spin-liquid compound ZnCu3(OD)6Cl2 (herbertsmithite) reveals in this paper antiferromagnetic correlations between impurity spins for energy transfers h(with stroke)ω < 0.8 meV (~ J/20). The momentum dependence differs significantly from higher energy scattering which arises from the intrinsic kagome spins. The low energy fluctuations are characterized by diffuse scattering near wave vectors (100) and (00 3/2), which is consistent with antiferromagnetic correlations between pairs of nearest-neighbor Cu impurities on adjacent triangular (Zn) interlayers. The corresponding impurity lattice resembles a simple cubic lattice in the dilute limit below the percolation threshold. Such an impurity model can describe prior neutron, NMR, and specific heat data. The low energy neutron data are consistent with the presence of a small spin gap (Δ ~ 0.7 meV) in the kagome layers, similar to that recently observed by NMR. Finally, the ability to distinguish the scattering due to Cu impurities from that of the planar kagome Cu spins provides an important avenue for probing intrinsic spin-liquid physics.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Univ. of Chicago, IL (United States). James Franck Inst. Dept. of Physics
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
- Stanford Univ., CA (United States). Dept. of Applied Physics; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Inst. for Materials and Energy Sciences
- National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). NIST Center for Neutron Research; Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science
- National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). NIST Center for Neutron Research; The United States Naval Academy, Annapolis, MD (United States). Dept. of Physics
- National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). NIST Center for Neutron Research; Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Physics and Astronomy. Inst. for Quantum Matter
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Johns Hopkins Univ., Baltimore, MD (United States); Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- Contributing Org.:
- Stanford Univ., CA (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States); The United States Naval Academy, Annapolis, MD (United States)
- OSTI Identifier:
- 1352675
- Alternate Identifier(s):
- OSTI ID: 1298336
- Grant/Contract Number:
- FG02-08ER46544; AC02-76SF00515; DMR-1508249
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 94; Journal Issue: 6; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; antiferromagnetism; frustrated magnetism; Kagome lattice; Heisenberg model; inelastic neutron scattering
Citation Formats
Han, Tian-Heng, Norman, M. R., Wen, J. -J., Rodriguez-Rivera, Jose A., Helton, Joel S., Broholm, Collin, and Lee, Young S. Correlated impurities and intrinsic spin-liquid physics in the kagome material herbertsmithite. United States: N. p., 2016.
Web. doi:10.1103/PhysRevB.94.060409.
Han, Tian-Heng, Norman, M. R., Wen, J. -J., Rodriguez-Rivera, Jose A., Helton, Joel S., Broholm, Collin, & Lee, Young S. Correlated impurities and intrinsic spin-liquid physics in the kagome material herbertsmithite. United States. https://doi.org/10.1103/PhysRevB.94.060409
Han, Tian-Heng, Norman, M. R., Wen, J. -J., Rodriguez-Rivera, Jose A., Helton, Joel S., Broholm, Collin, and Lee, Young S. Thu .
"Correlated impurities and intrinsic spin-liquid physics in the kagome material herbertsmithite". United States. https://doi.org/10.1103/PhysRevB.94.060409. https://www.osti.gov/servlets/purl/1352675.
@article{osti_1352675,
title = {Correlated impurities and intrinsic spin-liquid physics in the kagome material herbertsmithite},
author = {Han, Tian-Heng and Norman, M. R. and Wen, J. -J. and Rodriguez-Rivera, Jose A. and Helton, Joel S. and Broholm, Collin and Lee, Young S.},
abstractNote = {Low energy inelastic neutron scattering on single crystals of the kagome spin-liquid compound ZnCu3(OD)6Cl2 (herbertsmithite) reveals in this paper antiferromagnetic correlations between impurity spins for energy transfers h(with stroke)ω < 0.8 meV (~ J/20). The momentum dependence differs significantly from higher energy scattering which arises from the intrinsic kagome spins. The low energy fluctuations are characterized by diffuse scattering near wave vectors (100) and (00 3/2), which is consistent with antiferromagnetic correlations between pairs of nearest-neighbor Cu impurities on adjacent triangular (Zn) interlayers. The corresponding impurity lattice resembles a simple cubic lattice in the dilute limit below the percolation threshold. Such an impurity model can describe prior neutron, NMR, and specific heat data. The low energy neutron data are consistent with the presence of a small spin gap (Δ ~ 0.7 meV) in the kagome layers, similar to that recently observed by NMR. Finally, the ability to distinguish the scattering due to Cu impurities from that of the planar kagome Cu spins provides an important avenue for probing intrinsic spin-liquid physics.},
doi = {10.1103/PhysRevB.94.060409},
journal = {Physical Review B},
number = 6,
volume = 94,
place = {United States},
year = {Thu Aug 18 00:00:00 EDT 2016},
month = {Thu Aug 18 00:00:00 EDT 2016}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 86 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Spin chirality on a two-dimensional frustrated lattice
journal, March 2005
- Grohol, Daniel; Matan, Kittiwit; Cho, Jin-Hyung
- Nature Materials, Vol. 4, Issue 4
Low temperature magnetization of the kagome antiferromagnet
journal, October 2007
- Bert, F.; Nakamae, S.; Ladieu, F.
- Physical Review B, Vol. 76, Issue 13
On the crystal and magnetic ordering structures of clinoatacamite, γ-Cu 2 (OD) 3 Cl, a proposed valence bond solid
journal, November 2008
- Wills, A. S.; Henry, J-Y
- Journal of Physics: Condensed Matter, Vol. 20, Issue 47
Synthesis and characterization of single crystals of the spin- kagome-lattice antiferromagnets Zn Cu (OH) Cl
journal, March 2011
- Han, T. H.; Helton, J. S.; Chu, S.
- Physical Review B, Vol. 83, Issue 10
Topological excitations and the dynamic structure factor of spin liquids on the kagome lattice
journal, March 2014
- Punk, Matthias; Chowdhury, Debanjan; Sachdev, Subir
- Nature Physics, Vol. 10, Issue 4
Spin-Liquid Ground State of the S = 1/2 Kagome Heisenberg Antiferromagnet
journal, April 2011
- Yan, S.; Huse, D. A.; White, S. R.
- Science, Vol. 332, Issue 6034
Random Antiferromagnetic Chain
journal, November 1979
- Ma, Shang-keng; Dasgupta, Chandan; Hu, Chin-kun
- Physical Review Letters, Vol. 43, Issue 19
Dzyaloshinskii-Moriya interaction and spin reorientation transition in the frustrated kagome lattice antiferromagnet
journal, June 2011
- Matan, K.; Bartlett, B. M.; Helton, J. S.
- Physical Review B, Vol. 83, Issue 21
A Structurally Perfect S = 1 / 2 Kagomé Antiferromagnet
journal, October 2005
- Shores, Matthew P.; Nytko, Emily A.; Bartlett, Bart M.
- Journal of the American Chemical Society, Vol. 127, Issue 39
Dynamic Scaling in the Susceptibility of the Spin- Kagome Lattice Antiferromagnet Herbertsmithite
journal, April 2010
- Helton, J. S.; Matan, K.; Shores, M. P.
- Physical Review Letters, Vol. 104, Issue 14
Local spin susceptibility of the kagome lattice in ZnCu (OD) Cl
journal, July 2011
- Imai, T.; Fu, M.; Han, T. H.
- Physical Review B, Vol. 84, Issue 2
External Magnetic Field Effects on a Distorted Kagome Antiferromagnet
journal, September 2008
- Kim, J. -H.; Ji, S.; Lee, S. -H.
- Physical Review Letters, Vol. 101, Issue 10
Quantum Kagome Antiferromagnet ZnCu 3 (OH) 6 Cl 2
journal, January 2010
- Mendels, Philippe; Bert, Fabrice
- Journal of the Physical Society of Japan, Vol. 79, Issue 1
Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet
journal, December 2012
- Han, Tian-Heng; Helton, Joel S.; Chu, Shaoyan
- Nature, Vol. 492, Issue 7429
Evidence for a gapped spin-liquid ground state in a kagome Heisenberg antiferromagnet
journal, November 2015
- Fu, M.; Imai, T.; Han, T. -H.
- Science, Vol. 350, Issue 6261
, , and NMR in the Kagome Lattice
journal, February 2008
- Imai, T.; Nytko, E. A.; Bartlett, B. M.
- Physical Review Letters, Vol. 100, Issue 7
A temperature-induced reversible transformation between paratacamite and herbertsmithite
journal, September 2013
- Welch, Mark D.; Sciberras, Matthew J.; Williams, Peter A.
- Physics and Chemistry of Minerals, Vol. 41, Issue 1
Site Specific X-ray Anomalous Dispersion of the Geometrically Frustrated Kagomé Magnet, Herbertsmithite, ZnCu 3 (OH) 6 Cl 2
journal, November 2010
- Freedman, Danna E.; Han, Tianheng H.; Prodi, Andrea
- Journal of the American Chemical Society, Vol. 132, Issue 45
Density Matrix Renormalization Group Numerical Study of the Kagome Antiferromagnet
journal, September 2008
- Jiang, H. C.; Weng, Z. Y.; Sheng, D. N.
- Physical Review Letters, Vol. 101, Issue 11
Low-energy spin dynamics of the s = 1/2 kagome system herbertsmithite
journal, February 2013
- Nilsen, G. J.; de Vries, M. A.; Stewart, J. R.
- Journal of Physics: Condensed Matter, Vol. 25, Issue 10
Quantum kagome antiferromagnet : ZnCu 3 (OH) 6 Cl 2
journal, September 2011
- Mendels, Philippe; Bert, Fabrice
- Journal of Physics: Conference Series, Vol. 320
Refining the Spin Hamiltonian in the Spin- Kagome Lattice Antiferromagnet Using Single Crystals
journal, April 2012
- Han, Tianheng; Chu, Shaoyan; Lee, Young S.
- Physical Review Letters, Vol. 108, Issue 15
Magnetic structure of the kagomé lattice antiferromagnet potassium jarosite
journal, May 2000
- Inami, T.; Nishiyama, M.; Maegawa, S.
- Physical Review B, Vol. 61, Issue 18
Spin Dynamics of the Spin- Kagome Lattice Antiferromagnet
journal, March 2007
- Helton, J. S.; Matan, K.; Shores, M. P.
- Physical Review Letters, Vol. 98, Issue 10
Bond and site percolation in three dimensions
journal, May 2013
- Wang, Junfeng; Zhou, Zongzheng; Zhang, Wei
- Physical Review E, Vol. 87, Issue 5
Nature of the Spin-Liquid Ground State of the Heisenberg Model on the Kagome Lattice
journal, August 2012
- Depenbrock, Stefan; McCulloch, Ian P.; Schollwöck, Ulrich
- Physical Review Letters, Vol. 109, Issue 6
A Structurally Perfect S = 1/2 Kagome Antiferromagnet.
journal, December 2005
- Shores, Matthew P.; Nytko, Emily A.; Bartlett, Bart M.
- ChemInform, Vol. 36, Issue 50
Random Antiferromagnetic Chain.
journal, December 1979
- Ma, Shang-keng; Dasgupta, Chandan; Hu, Chin-kun
- Physical Review Letters, Vol. 43, Issue 25
External magnetic field effects on a distorted kagome antiferromagnet
text, January 2008
- Kim, J. -H.; Ji, S.; Lee, S. -H.
- arXiv
Dzyaloshinskii-Moriya interaction and spin re-orientation transition in the frustrated kagome lattice antiferromagnet
text, January 2011
- Matan, K.; Bartlett, B. M.; Helton, J. S.
- arXiv
Bond and Site Percolation in Three Dimensions
text, January 2013
- Wang, Junfeng; Zhou, Zongzheng; Zhang, Wei
- arXiv
Evidence for a Gapped Spin-Liquid Ground State in a Kagome Heisenberg Antiferromagnet
text, January 2015
- Fu, M.; Imai, T.; Han, T. -H.
- arXiv
Works referencing / citing this record:
Tuning of a Kagome Magnet: Insulating Ground State in Ga‐Substituted Cu 4 (OH) 6 Cl 2
journal, February 2019
- Puphal, Pascal; Ranjith, Kizhake Malayil; Pustogow, Andrej
- physica status solidi (b), Vol. 256, Issue 9
Theoretical and experimental developments in quantum spin liquid in geometrically frustrated magnets: a review
journal, November 2019
- Shaginyan, V. R.; Stephanovich, V. A.; Msezane, A. Z.
- Journal of Materials Science, Vol. 55, Issue 6
Scaling and data collapse from local moments in frustrated disordered quantum spin systems
journal, October 2018
- Kimchi, Itamar; Sheckelton, John P.; McQueen, Tyrel M.
- Nature Communications, Vol. 9, Issue 1
Synthetic investigation of competing magnetic interactions in 2D metal–chloranilate radical frameworks
journal, January 2020
- Collins, Kelsey A.; Saballos, Richard J.; Fataftah, Majed S.
- Chemical Science
Quantum magnetism in minerals
journal, July 2018
- Inosov, D. S.
- Advances in Physics, Vol. 67, Issue 3
Quantum spin liquids: a review
journal, November 2016
- Savary, Lucile; Balents, Leon
- Reports on Progress in Physics, Vol. 80, Issue 1
Functional renormalization group for frustrated magnets with nondiagonal spin interactions
journal, September 2019
- Buessen, Finn Lasse; Noculak, Vincent; Trebst, Simon
- Physical Review B, Vol. 100, Issue 12
Theory of quantum kagome ice and vison zero modes
journal, February 2017
- Huang, Yi-Ping; Hermele, Michael
- Physical Review B, Vol. 95, Issue 7
Rapid filling of the spin gap with temperature in the Schwinger-boson mean-field theory of the antiferromagnetic Heisenberg kagome model
journal, April 2019
- Halimeh, Jad C.; Singh, Rajiv R. P.
- Physical Review B, Vol. 99, Issue 15
Diagnosing Fractionalization from the Spin Dynamics of Spin Liquids on the Kagome Lattice by Quantum Monte Carlo Simulations
journal, August 2018
- Becker, Jonas; Wessel, Stefan
- Physical Review Letters, Vol. 121, Issue 7
Choreographed entanglement dances: Topological states of quantum matter
journal, February 2019
- Wen, Xiao-Gang
- Science, Vol. 363, Issue 6429
Quantum spin liquids
journal, January 2020
- Broholm, C.; Cava, R. J.; Kivelson, S. A.
- Science, Vol. 367, Issue 6475
Thermodynamic, Dynamic, and Transport Properties of Quantum Spin Liquid in Herbertsmithite from an Experimental and Theoretical Point of View
journal, August 2019
- Shaginyan, Vasily R.; Msezane, Alfred Z.; Amusia, Miron Ya.
- Condensed Matter, Vol. 4, Issue 3
Functional renormalization group for frustrated magnets with nondiagonal spin interactions
text, January 2019
- Buessen, Finn Lasse; Noculak, Vincent; Trebst, Simon
- Freie Universität Berlin
Spin structure factors of chiral quantum spin liquids on the kagome lattice
text, January 2016
- Halimeh, Jad C.; Punk, Matthias
- arXiv
Gapped spin-1/2 spinon excitations in a new kagome quantum spin liquid compound Cu$_3$Zn(OH)$_6$FBr
text, January 2017
- Feng, Zili; Li, Zheng; Meng, Xin
- arXiv
Nature of the spin liquid ground state in a breathing kagome compound studied by NMR and series expansion
text, January 2017
- Orain, J. -C.; Bernu, B.; Mendels, P.
- arXiv
Scaling and data collapse from local moments in frustrated disordered quantum spin systems
text, January 2018
- Kimchi, Itamar; Sheckelton, John P.; McQueen, Tyrel M.
- arXiv
From Claringbullite to a new spin liquid candidate Cu$_3$Zn(OH)$_6$FCl
text, January 2018
- Feng, Zili; Yi, Wei; Zhu, Kejia
- arXiv
Rapid filling of the spin gap with temperature in the Schwinger-boson mean-field theory of the antiferromagnetic Heisenberg kagome model
text, January 2018
- Halimeh, Jad C.; Singh, Rajiv R. P.
- arXiv
Gapless spin liquid in the kagome Heisenberg antiferromagnet with Dzyaloshinskii-Moriya interactions
text, January 2018
- Lee, Chih-Yuan; Normand, B.; Kao, Ying-Jer
- arXiv
Choreographed entangle dances: topological states of quantum matter
text, January 2019
- Wen, Xiao-Gang
- arXiv