- Open Access
Anharmonic quantum effects of implanted muons: Route to probing nuclear quantum behavior in solids
Phys. Rev. B 113, 224420 – Published 8 June, 2026
DOI: https://doi.org/10.1103/x1y3-9chs
Abstract
The quantum behavior of light particles in solids gives rise to phenomena that cannot be captured by a classical description. We show that muon spin spectroscopy (), when paired with a quantum-mechanical treatment of the implanted muon, becomes a sensitive and direct probe of nuclear quantum effects. By modeling the muon as a spatially extended quantum particle, our approach captures strong anharmonic behavior. We demonstrate this in Zn-barlowite, which serves as a nontrivial test case due to its structurally complex lattice and the presence of both fluorine and hydroxyl groups. Our results establish a route for extracting nuclear quantum signatures from data and open different opportunities for studying light nuclei such as hydrogen and lithium in systems where quantum fluctuations shape structure and function.
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References (47)
- T. E. Markland and M. Ceriotti, Nuclear quantum effects enter the mainstream, Nat. Rev. Chem. 2, 0109 (2018).
- U. Ranieri, L. J. Conway, M.-E. Donnelly, H. Hu, M. Wang, P. Dalladay-Simpson, M. Peña-Alvarez, E. Gregoryanz, A. Hermann, and R. T. Howie, Formation and stability of dense methane-hydrogen compounds, Phys. Rev. Lett. 128, 215702 (2022).
- G. J. Ackland, M. Dunuwille, M. Martinez-Canales, I. Loa, R. Zhang, S. Sinogeikin, W. Cai, and S. Deemyad, Quantum and isotope effects in lithium metal, Science 356, 1254 (2017).
- A. Drozdov, M. Eremets, I. Troyan, V. Ksenofontov, and S. I. Shylin, Conventional superconductivity at 203 kelvin at high pressures in the sulfur hydride system, Nature (London) 525, 73 (2015).
- M. I. Eremets, V. S. Minkov, A. P. Drozdov, P. Kong, V. Ksenofontov, S. I. Shylin, S. L. Bud'ko, R. Prozorov, F. F. Balakirev, D. Sun, et al., High-temperature superconductivity in hydrides: Experimental evidence and details, J. Supercond. Novel Magn. 35, 965 (2022).
- M. Rossi, P. Gasparotto, and M. Ceriotti, Anharmonic and quantum fluctuations in molecular crystals: A first-principles study of the stability of paracetamol, Phys. Rev. Lett. 117, 115702 (2016).
- Y. Litman, V. Kapil, Y. M. Y. Feldman, D. Tisi, T. Begušić, K. Fidanyan, G. Fraux, J. Higer, M. Kellner, T. E. Li, E. S. Pós, E. Stocco, G. Trenins, B. Hirshberg, M. Rossi, and M. Ceriotti, i-pi 3.0: A flexible and efficient framework for advanced atomistic simulations, J. Chem. Phys. 161, 062504 (2024).
- S. J. Blundell, R. De Renzi, T. Lancaster, and F. L. Pratt, Muon Spectroscopy: An Introduction (Oxford University Press, Oxford, UK, 2021).
- A. Yaouanc and P. D. De Reotier, Muon Spin Rotation, Relaxation, and Resonance: Applications to Condensed Matter, International Series of Monographs on Physics No. 147 (Oxford University Press, Oxford, UK, 2011).
- A. Amato and E. Morenzoni, Introduction to Muon Spin Spectroscopy: Applications to Solid State and Material Sciences (Springer, Berlin, 2024).
- J. S. Möller, D. Ceresoli, T. Lancaster, N. Marzari, and S. J. Blundell, Quantum states of muons in fluorides, Phys. Rev. B 87, 121108(R) (2013).
- S. Blundell and T. Lancaster, : Density functional theory for muon site determination, Appl. Phys. Rev. 10, 021316 (2023).
- A. Amato, P. Dalmas de Réotier, D. Andreica, A. Yaouanc, A. Suter, G. Lapertot, I. M. Pop, E. Morenzoni, P. Bonfà, F. Bernardini, and R. De Renzi, Understanding the spectra of MnSi without magnetic polarons, Phys. Rev. B 89, 184425 (2014).
- F. R. Foronda, F. Lang, J. S. Möller, T. Lancaster, A. T. Boothroyd, F. L. Pratt, S. R. Giblin, D. Prabhakaran, and S. J. Blundell, Anisotropic local modification of crystal field levels in Pr-based pyrochlores: A muon-induced effect modeled using density functional theory, Phys. Rev. Lett. 114, 017602 (2015).
- M. Gomilšek, F. L. Pratt, S. P. Cottrell, S. J. Clark, and T. Lancaster, Many-body quantum muon effects and quadrupolar coupling in solids, Commun. Phys. 6, 142 (2023).
- I. J. Onuorah, P. Bonfà, R. De Renzi, L. Monacelli, F. Mauri, M. Calandra, and I. Errea, Quantum effects in muon spin spectroscopy within the stochastic self-consistent harmonic approximation, Phys. Rev. Mater. 3, 073804(R) (2019).
- S. Mañas-Valero, B. M. Huddart, T. Lancaster, E. Coronado, and F. L. Pratt, Quantum phases and spin liquid properties of 1T-, npj Quantum Mater. 6, 69 (2021).
- 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).
- J. Wang, W. Yuan, P. M. Singer, R. W. Smaha, W. He, J. Wen, Y. S. Lee, and T. Imai, Freezing of the lattice in the kagome lattice Heisenberg antiferromagnet Zn-barlowite (OD), Phys. Rev. Lett. 128, 157202 (2022).
- Z. Feng, Z. Li, X. Meng, W. Yi, Y. Wei, J. Zhang, Y.-C. Wang, W. Jiang, Z. Liu, S. Li, et al., Gapped spin-1/2 spinon excitations in a new kagome quantum spin liquid compound (OH), Chin. Phys. Lett. 34, 077502 (2017).
- 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).
- L. Savary and L. Balents, Quantum spin liquids: A review, Rep. Prog. Phys. 80, 016502 (2017).
- P. Mendels and F. Bert, Quantum kagome frustrated antiferromagnets: One route to quantum spin liquids, C. R. Phys. 17, 455 (2016).
- C. Broholm, R. J. Cava, S. A. Kivelson, D. G. Nocera, M. R. Norman, and T. Senthil, Quantum spin liquids, Science 367, eaay0668 (2020).
- J. Wang, W. Yuan, P. M. Singer, A. Schneidewind, D. T. Adroja, A. Zorko, J. G. Cheng, and M. Fu, Emergence of spin singlets with inhomogeneous gaps in the kagome lattice Heisenberg antiferromagnets Zn-barlowite and herbertsmithite, Nat. Phys. 17, 1109 (2021).
- S. Yan, D. A. Huse, and S. R. White, Spin-liquid ground state of the kagome Heisenberg antiferromagnet, Science 332, 1173 (2011).
- J. Khatua, B. Sana, A. Zorko, M. Gomilšek, K. Sethupathi, M. R. Rao, M. Baenitz, B. Schmidt, and P. Khuntia, Experimental signatures of quantum and topological states in frustrated magnetism, Phys. Rep. 1041, 1 (2023).
- B. Huddart, A. Hernández-Melián, T. Hicken, M. Gomilšek, Z. Hawkhead, S. Clark, F. Pratt, and T. Lancaster, Mufinder: A program to determine and analyse muon stopping sites, Comput. Phys. Commun. 280, 108488 (2022).
- S. Baroni, S. de Gironcoli, A. Dal Corso, and P. Giannozzi, Phonons and related crystal properties from density-functional perturbation theory, Rev. Mod. Phys. 73, 515 (2001).
- J. S. Lord, Computer simulation of muon spin evolution, Physica B 374-375, 472 (2006).
- J. S. Lord, S. Cottrell, and W. Williams, Muon spin relaxation in strongly coupled systems, Physica B 289-290, 495 (2000).
- J. M. Wilkinson and S. J. Blundell, Information and decoherence in a muon-fluorine coupled system, Phys. Rev. Lett. 125, 087201 (2020).
- M. Celio, New method to calculate the muon polarization function, Phys. Rev. Lett. 56, 2720 (1986).
- P. Bonfà, J. Frassineti, J. M. Wilkinson, G. Prando, M. M. Isah, C. Wang, T. Spina, B. Joseph, V. F. Mitrović, R. De Renzi, S. J. Blundell, and S. Sanna, Entanglement between muon and nuclear spins as a probe of charge environment, Phys. Rev. Lett. 129, 097205 (2022).
- R. Wang, X. Li, X. Han, J. Lin, Y. Wang, T. Qian, H. Ding, Y. Shi, and X. Liu, X-ray absorption investigation of the site occupancies of the copper element in nominal (OH), Chin. Phys. B 30, 046102 (2021).
- R. S. Hayano, Y. J. Uemura, J. Imazato, N. Nishida, T. Yamazaki, and R. Kubo, Zero-and low-field spin relaxation studied by positive muons, Phys. Rev. B 20, 850 (1979).
- https://musruser.psi.ch/cgi-bin/SearchDB.cgi
- S. J. Clark, M. D. Segall, C. J. Pickard, P. J. Hasnip, M. I. J. Probert, K. Refson, and M. C. Payne, First principles methods using CASTEP, Z. Kristallogr. - Cryst. Mater. 220, 567 (2005).
- T. Björkman, CIF2Cell: Generating geometries for electronic structure programs, Comput. Phys. Commun. 182, 1183 (2011).
- J. P. Perdew, A. Ruzsinszky, G. I. Csonka, O. A. Vydrov, G. E. Scuseria, L. A. Constantin, X. Zhou, and K. Burke, Restoring the density-gradient expansion for exchange in solids and surfaces, Phys. Rev. Lett. 100, 136406 (2008).
- H. J. Monkhorst and J. D. Pack, Special points for Brillouin-zone integrations, Phys. Rev. B 13, 5188 (1976).
- V. I. Anisimov, J. Zaanen, and O. K. Andersen, Band theory and Mott insulators: Hubbard U instead of stoner I, Phys. Rev. B 44, 943 (1991).
- D. Guterding, R. Valentí, and H. O. Jeschke, Reduction of magnetic interlayer coupling in barlowite through isoelectronic substitution, Phys. Rev. B 94, 125136 (2016).
- H. O. Jeschke, F. Salvat-Pujol, E. Gati, N. H. Hoang, B. Wolf, M. Lang, J. A. Schlueter, and R. Valentí, Barlowite as a canted antiferromagnet: Theory and experiment, Phys. Rev. B 92, 094417 (2015).
- W. Kohn and L. J. Sham, Self-consistent equations including exchange and correlation effects, Phys. Rev. 140, A1133 (1965).
- J. P. Perdew, K. Burke, and Y. Wang, Generalized gradient approximation for the exchange-correlation hole of a many-electron system, Phys. Rev. B 54, 16533 (1996).
- M. Newville, T. Stensitzki, D. B. Allen, M. Rawlik, A. Ingargiola, and A. Nelson, LMFIT: Non-linear least-square minimization and curve-fitting for Python, Astrophys. Source Code Lib. ascl (2016).