- Open Access
Fluctuating magnetism in Zn-doped averievite with well-separated kagome layers
Phys. Rev. Materials 9, 074003 – Published 11 July, 2025
DOI: https://doi.org/10.1103/l7gq-cc96
Abstract
Kagome lattice decorated with spins is one of the most discussed ways to realize a quantum spin liquid. However, all previous material realizations of this model have suffered from additional complications, ranging from additional interactions to impurity effects. Recently, a new quantum kagome system has been identified in the form of averievite (CsCl), featuring a unique double-layer spacing between the kagome planes. Using muon spin spectroscopy we show that only a complete substitution (i.e., ) of interplanar copper ions leads to a quantum-disordered ground state. In contrast, the parent compound () exhibits long-range magnetic order, with a phase transition around 24 K. Experiments performed on the partially substituted material () show that the transformation proceeds through an intermediate disordered, partially frozen ground state, unaffected by pressures up to 23 kbar. Our study provides a microscopic view of the magnetism of the decoupling of the kagome layers and establishes the averievite as a new material platform for the experimental study of the fully-decoupled kagome layers.
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References (49)
- P. W. Anderson, Resonating valence bonds: A new kind of insulator? Mater. Res. Bull. 8, 153 (1973).
- P. W. Anderson, The resonating valence bond state in and superconductivity, Science 235, 1196 (1987).
- L. Balents, Spin liquids in frustrated magnets, Nature (London) 464, 199 (2010).
- L. Savary and L. Balents, Quantum spin liquids: A review, Rep. Prog. Phys. 80, 016502 (2017).
- C. Broholm, R. J. Cava, S. A. Kivelson, D. G. Nocera, M. R. Norman, and T. Senthil, Quantum spin liquids, Science 367, eaay0668 (2020).
- M. B. Hastings, Dirac structure, RVB, and Goldstone modes in the kagomé antiferromagnet, Phys. Rev. B 63, 014413 (2000).
- Y. Ran, M. Hermele, P. A. Lee, and X.-G. Wen, Projected-wave-function study of the spin- Heisenberg model on the kagomé lattice, Phys. Rev. Lett. 98, 117205 (2007).
- O. Cépas, C. M. Fong, P. W. Leung, and C. Lhuillier, Quantum phase transition induced by Dzyaloshinskii-Moriya interactions in the kagome antiferromagnet, Phys. Rev. B 78, 140405(R) (2008).
- C.-Y. Lee, B. Normand, and Y.-J. Kao, Gapless spin liquid in the kagome Heisenberg antiferromagnet with Dzyaloshinskii-Moriya interactions, Phys. Rev. B 98, 224414 (2018).
- H. C. Jiang, Z. Y. Weng, and D. N. Sheng, Density matrix renormalization group numerical study of the kagome antiferromagnet, Phys. Rev. Lett. 101, 117203 (2008).
- S. Yan, D. A. Huse, and S. R. White, Spin-liquid ground state of the kagome Heisenberg antiferromagnet, Science 332, 1173 (2011).
- S. Depenbrock, I. P. McCulloch, and U. Schollwöck, Nature of the spin-liquid ground state of the Heisenberg model on the kagome lattice, Phys. Rev. Lett. 109, 067201 (2012).
- Y. Iqbal, F. Becca, S. Sorella, and D. Poilblanc, Gapless spin-liquid phase in the kagome spin- Heisenberg antiferromagnet, Phys. Rev. B 87, 060405(R) (2013).
- Y. Iqbal, D. Poilblanc, and F. Becca, Spin- Heisenberg antiferromagnet on the kagome lattice, Phys. Rev. B 91, 020402(R) (2015).
- H. J. Liao, Z. Y. Xie, J. Chen, Z. Y. Liu, H. D. Xie, R. Z. Huang, B. Normand, and T. Xiang, Gapless spin-liquid ground state in the kagome antiferromagnet, Phys. Rev. Lett. 118, 137202 (2017).
- M. P. Shores, E. A. Nytko, B. M. Bartlett, and D. G. Nocera, A structurally perfect kagomé antiferromagnet, J. Am. Chem. Soc. 127, 13462 (2005).
- P. Mendels, F. Bert, M. A. de Vries, A. Olariu, A. Harrison, F. Duc, J. C. Trombe, J. S. Lord, A. Amato, and C. Baines, Quantum magnetism in the paratacamite family: Towards an ideal kagomé lattice, Phys. Rev. Lett. 98, 077204 (2007).
- K. Tustain, B. Ward-O'Brien, F. Bert, T. Han, H. Luetkens, T. Lancaster, B. M. Huddart, P. J. Baker, and L. Clark, From magnetic order to quantum disorder in the Zn-barlowite series of kagomé antiferromagnets, npj Quantum Mater. 5, 74 (2020).
- R. W. Smaha, W. He, J. M. Jiang, J. Wen, Y.-F. Jiang, J. P. Sheckelton, C. J. Titus, S. G. Wang, Y.-S. Chen, S. J. Teat, A. A. Aczel, Y. Zhao, G. Xu, J. W. Lynn, H.-C. Jiang, and Y. S. Lee, Materializing rival ground states in the barlowite family of kagome magnets: Quantum spin liquid, spin ordered, and valence bond crystal states, npj Quantum Mater. 5, 23 (2020).
- P. Khuntia, M. Velazquez, Q. Barthélemy, F. Bert, E. Kermarrec, A. Legros, B. Bernu, L. Messio, A. Zorko, and P. Mendels, Gapless ground state in the archetypal quantum kagome antiferromagnet , Nat. Phys. 16, 469 (2020).
- J. Wang, W. Yuan, P. M. Singer, R. W. Smaha, W. He, J. Wen, Y. S. Lee, and T. Imai, Emergence of spin singlets with inhomogeneous gaps in the kagome lattice Heisenberg antiferromagnets Zn-barlowite and herbertsmithite, Nat. Phys. 17, 1109 (2021).
- T.-H. Han, J. S. Helton, S. Chu, D. G. Nocera, J. A. Rodriguez-Rivera, C. Broholm, and Y. S. Lee, Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet, Nature (London) 492, 406 (2012).
- T.-H. Han, M. R. Norman, J.-J. Wen, J. A. Rodriguez-Rivera, J. S. Helton, C. Broholm, and Y. S. Lee, Correlated impurities and intrinsic spin-liquid physics in the kagome material herbertsmithite, Phys. Rev. B 94, 060409(R) (2016).
- M. Punk, D. Chowdhury, and S. Sachdev, Topological excitations and the dynamic structure factor of spin liquids on the kagome lattice, Nat. Phys. 10, 289 (2014).
- A. T. Breidenbach, A. C. Campello, J. Wen, H.-C. Jiang, D. M. Pajerowski, R. W. Smaha, and Y. S. Lee, Identifying universal spin excitations in spin- kagome quantum spin liquid materials, arXiv:2504.06491.
- L. P. Vergasova, G. L. Starova, S. K. Filatov, and V. V. Anan'ev, Averievite ()—A new mineral of volcanic exhalations, Dokl. Earth Sci. 359, 804 (1998).
- A. S. Botana, H. Zheng, S. H. Lapidus, J. F. Mitchell, and M. R. Norman, Averievite: A copper oxide kagome antiferromagnet, Phys. Rev. B 98, 054421 (2018).
- T. Biesner, S. Roh, A. Pustogow, H. Zheng, J. F. Mitchell, and M. Dressel, Magnetic terahertz resonances above the Néel temperature in the frustrated kagome antiferromagnet averievite, Phys. Rev. B 105, L060410 (2022).
- C. Liu, C. Ma, T. Chang, X. Wang, C. Fan, L. Han, F. Li, S. Wang, Y.-S. Chen, and J. Zhang, Bulk crystal growth and single-crystal-to-single-crystal phase transitions in the averievite , Cryst. Growth Des. 24, 9701 (2024).
- M. Georgopoulou, D. Boldrin, B. Fåk, P. Manuel, A. Gibbs, J. Ollivier, E. Suard, and A. S. Wills, Magnetic ground states and excitations in Zn-doped averieite – A family of oxide-based kagome antiferromagnets, arXiv:2306.14739.
- A. Amato, H. Luetkens, K. Sedlak, A. Stoykov, R. Scheuermann, M. Elender, A. Raselli, and D. Graf, The new versatile general purpose surface-muon instrument (GPS) based on silicon photomultipliers for measurements on a continuous-wave beam, Rev. Sci. Instrum. 88, 093301 (2017).
- R. Khasanov, Z. Guguchia, A. Maisuradze, D. Andreica, M. Elender, A. Raselli, Z. Shermadini, T. Goko, F. Knecht, E. Morenzoni, and A. Amato, High pressure research using muons at the Paul Scherrer Institute, High Press. Res. 36, 140 (2016).
- Z. Shermadini, R. Khasanov, M. Elender, G. Simutis, Z. Guguchia, K. V. Kamenev, and A. Amato, A low-background piston-cylinder-type hybrid high-pressure cell for muon-spin rotation/relaxation experiments, High Press. Res. 37, 449 (2017).
- A. Suter and B. Wojek, Musrfit: A free platform-independent framework for data analysis, Phys. Procedia 30, 69 (2012).
- S. Guchhait, D. V. Ambika, S. Mohanty, Y. Furukawa, and R. Nath, Magnetic properties of the frustrated spin- capped-kagome antiferromagnet (CsBr), Phys. Rev. B 110, 174447 (2024).
- K. Somesh, Y. Furukawa, G. Simutis, F. Bert, M. Prinz-Zwick, N. Büttgen, A. Zorko, A. A. Tsirlin, P. Mendels, and R. Nath, Universal fluctuating regime in triangular chromate antiferromagnets, Phys. Rev. B 104, 104422 (2021).
- E. Kermarrec, P. Mendels, F. Bert, R. H. Colman, A. S. Wills, P. Strobel, P. Bonville, A. Hillier, and A. Amato, Spin-liquid ground state in the frustrated kagome antiferromagnet (OH), Phys. Rev. B 84, 100401(R) (2011).
- L. Clark, J. C. Orain, F. Bert, M. A. De Vries, F. H. Aidoudi, R. E. Morris, P. Lightfoot, J. S. Lord, M. T. F. Telling, P. Bonville, J. P. Attfield, P. Mendels, and A. Harrison, Gapless spin liquid ground state in the vanadium oxyfluoride kagome antiferromagnet , Phys. Rev. Lett. 110, 207208 (2013).
- Y. Li, D. Adroja, P. K. Biswas, P. J. Baker, Q. Zhang, J. Liu, A. A. Tsirlin, P. Gegenwart, and Q. Zhang, Muon spin relaxation evidence for the (1) quantum spin-liquid ground state in the triangular antiferromagnet , Phys. Rev. Lett. 117, 097201 (2016).
- M. Majumder, G. Simutis, I. E. Collings, J.-C. Orain, T. Dey, Y. Li, P. Gegenwart, and A. A. Tsirlin, Persistent spin dynamics in the pressurized spin-liquid candidate , Phys. Rev. Res. 2, 023191 (2020).
- D. R. Noakes and G. M. Kalvius, Anomalous zero-field muon spin relaxation in highly disordered magnets, Phys. Rev. B 56, 2352 (1997).
- Y. Alexanian, R. Kumar, H. Zeroual, B. Bernu, L. Mangin-Thro, J. R. Stewart, J. M. Wilkinson, S. Bhattacharya, P. L. Paulose, F. Bert, P. Mendels, B. Fåk, and E. Kermarrec, Three-dimensional spin liquid state in the frustrated Heisenberg garnet , Phys. Rev. Materials (2025).
- Y. J. Uemura, A. Keren, K. Kojima, L. P. Le, G. M. Luke, W. D. Wu, Y. Ajiro, T. Asano, Y. Kuriyama, M. Mekata, H. Kikuchi, and K. Kakurai, Spin fluctuations in frustrated kagomé lattice system studied by muon spin relaxation, Phys. Rev. Lett. 73, 3306 (1994).
- E. Kermarrec, J. Gaudet, K. Fritsch, R. Khasanov, Z. Guguchia, C. Ritter, K. A. Ross, H. A. Dabkowska, and B. D. Gaulin, Ground state selection under pressure in the quantum pyrochlore magnet , Nat. Commun. 8, 14810 (2017).
- M. Majumder, R. S. Manna, G. Simutis, J. C. Orain, T. Dey, F. Freund, A. Jesche, R. Khasanov, P. K. Biswas, E. Bykova, N. Dubrovinskaia, L. S. Dubrovinsky, R. Yadav, L. Hozoi, S. Nishimoto, A. A. Tsirlin, and P. Gegenwart, Breakdown of magnetic order in the pressurized kitaev iridate , Phys. Rev. Lett. 120, 237202 (2018).
- D. Chatterjee, P. Doležal, F. Abbruciati, T. Biesner, K. M. Zoch, R. Khasanov, S. S. Islam, G. Kaur, S. Roh, F. Capitani, G. Garbarino, C. Krellner, P. Mendels, E. Kermarrec, M. Dressel, B. Wehinger, A. Pustogow, F. Bert, and P. Puphal, Spin liquid state in Y-kapellasite, (OH) by external pressure controlled frustration, arXiv:2502.09733.
- M. R. Norman, Colloquium: Herbertsmithite and the search for the quantum spin liquid, Rev. Mod. Phys. 88, 041002 (2016).
- T.-H. Han, J. Singleton, and J. A. Schlueter, Barlowite: A spin- antiferromagnet with a geometrically perfect kagome motif, Phys. Rev. Lett. 113, 227203 (2014).
- W. Yuan, J. Wang, P. M. Singer, R. W. Smaha, J. Wen, Y. S. Lee, and T. Imai, Emergence of the spin polarized domains in the kagome lattice Heisenberg antiferromagnet Zn-barlowite ()(OD), npj Quantum Mater. 7, 120 (2022).