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TlYbSe2 as a member of the J=12 triangular-lattice Yb delafossite family: From spin liquid to field-induced magnetic order

T. Fujii1, M. Pillaca2, F. Bärtl3,4, J. Sichelschmidt1, S. Luther3, H. Rosner1, A. M. Strydom5, J. Wosnitza3,4, H. Kühne3 et al.

Th. Doert2 and M. Baenitz1,*

  • *Contact author: michael.baenitz@cpfs.mpg.de
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Phys. Rev. B 112, 024426 – Published 18 July, 2025

DOI: https://doi.org/10.1103/lkqb-3fc7

Abstract

TlYbSe2 is a new member of the Yb delafossite family, which differs strongly from the previously investigated alkali-metal Yb delafossites. It is characterized by a much larger saturation field (about 20 T) and a higher transition temperature (about 1.8 K) to the field-induced ordered state. As for the other Yb delafossites, long-range magnetic order is absent down to low temperatures at zero field. We report detailed macroscopic and microscopic measurements as a function of magnetic field and temperature to explore the H−T phase diagram of polycrystalline TlYbSe2. Besides bulk methods, such as magnetization and specific heat, spectroscopic methods, such as electron spin resonance (ESR) and nuclear magnetic resonance (NMR), are applied. The magnetic anisotropy can be determined by means of these microscopic probes; in particular, Yb-ESR and Se-NMR are powerful tools here. The magnetization, ESR, and NMR data evidence a large anisotropy factor of about 10 for the ratio of the magnetic moment in the Yb-Se triangular-lattice plane and perpendicular to it. Such a strong spin anisotropy was only found in CsYbSe2, which identifies both systems as prototype two-dimensional triangular-lattice spin liquids. Even though CsYbSe2 shares the same spin anisotropy, it has a much smaller magnetic exchange coupling between the Yb moments than TlYbSe2, which leads to a field-induced ordering at much lower temperatures (1 K) and a smaller saturation field of only 10 T. We speculate that this originates from the use of thallium as a monovalent cation (Tl+1 with [Xe]4f145d106s2) instead of the intensively studied alkali metals (Na+1, K+1, Rb+1, Cs+1) with completely filled (Ne, Ar, Kr, Xe) shells. In particular, the emergence of a Tl+1-based lone-pair 6s2−Se−4p polarization might have a strong impact on the strength and anisotropy of the magnetic exchange among the Yb ions in the TlYbSe2 lattice. In contrast to that, the spin anisotropy of the pseudo-spin-1/2 Yb ions remains unaltered by the presence of Tl 6s2 lone pairs.

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References (38)

  1. M. A. Marquardt, N. A. Ashmore, and D. P. Cann, Crystal chemistry and electrical properties of the delafossite structure, Thin Solid Films 496, 146 (2006).
  2. A. P. Mackenzie, The properties of ultrapure delafossite metals, Rep. Prog. Phys. 80, 032501 (2017).
  3. J. P. Doumerc, A. Wichainchai, A. Ammar, M. Pouchard, and P. Hagenmuller, On magnetic-properties of some oxides with delafossite-type structure, Mater. Res. Bull. 21, 745 (1986).
  4. A. P. Ramirez, Geometrical frustration, Handbook Magnet. Mater. 13, 423 (2001), Chap. 4.
  5. M. Baenitz, Ph. Schlender, J. Sichelschmidt, Y. A. Onykiienko, Z. Zangeneh, K. M. Ranjith, R. Sarkar, L. Hozoi, H. C. Walker, J. C. Orain, H. Yasuoka, J. van den Brink, H. H. Klauss, D. S. Inosov, and Th. Doert, NaYbS2: A planar spin-1/2 triangular-lattice magnet and putative spin liquid, Phys. Rev. B 98, 220409 (2018).
  6. K. M. Ranjith, D. Dmytriieva, S. Khim, J. Sichelschmidt, S. Luther, D. Ehlers, H. Yasuoka, J. Wosnitza, A. A. Tsirlin, H. Kühne, and M. Baenitz, Field-induced instability of the quantum spin liquid ground state in the Jeff=1/2 triangular-lattice compound NaYbO2, Phys. Rev. B 99, 180401(R) (2019).
  7. K. M. Ranjith, S. Luther, T. Reimann, B. Schmidt, Ph. Schlender, J. Sichelschmidt, H. Yasuoka, A. M. Strydom, Y. Skourski, J. Wosnitza, H. Kühne, Th. Doert, and M. Baenitz, Anisotropic field-induced ordering in the triangular-lattice quantum spin liquid NaYbSe2, Phys. Rev. B 100, 224417 (2019).
  8. W. Liu, Z. Zhang, J. Ji, Y. Liu, J. Li, X. Wang, H. Lei, G. Chen, and Q. Zhang, Rare-earth chalcogenides: A large family of triangular lattice spin liquid candidates, Chin. Phys. Lett. 35, 117501 (2018).
  9. B. Schmidt, J. Sichelschmidt, K. M. Ranjith, Th. Doert, and M. Baenitz, Yb delafossites: Unique exchange frustration of 4f spin-1/2 moments on a perfect triangular lattice, Phys. Rev. B 103, 214445 (2021).
  10. M. Xie, W. Zhuo, Y. Cai, Z. Zhang, and Q. Zhang, Rare-earth chalcogenides: An inspiring playground for exploring frustrated magnetism, Chin. Phys. Lett. 41, 117505 (2024).
  11. A. V. Chubukov and D. I. Golosov, Quantum-theory of an antiferromagnet on a triangular lattice in a magnetic-field, J. Phys.: Condens. Matter 3, 69 (1991).
  12. T. Xie, A. A. Eberharter, J. Xing, S. Nishimoto, M. Brando, P. Khanenko, J. Sichelschmidt, A. A. Turrini, D. G. Mazzone, P. G. Naumov, L. D. Sanjeewa, N. Harrison, A. S. Sefat, B. Normand, A. M. Laeuchli, A. Podlesnyak, and S. E. Nikitin, Complete field-induced spectral response of the spin-1/2 triangular-lattice antiferromagnet CsYbSe2, npj Quantum Mater. 8, 48 (2023).
  13. J. Xing, L. D. Sanjeewa, J. Kim, G. R. Stewart, M.-H. Du, F. A. Reboredo, R. Custelcean, and A. S. Sefat, Crystal synthesis and frustrated magnetism in triangular lattice CsRESe2 (RE = La-Lu): Quantum spin liquid candidates CsCeSe2 and CsYbSe2, ACS Mater. Lett. 2, 71 (2020).
  14. T. Ferreira, J. Xing, L. D. Sanjeewa, and A. S. Sefat, Frustrated magnetism in triangular lattice TlYbS2 crystals grown via molten flux, Front. Chem. 8, 00127 (2020).
  15. Y. Skourski, M. D. Kuz'min, K. P. Skokov, A. V. Andreev, and J. Wosnitza, High-field magnetization of Ho2Fe17, Phys. Rev. B 83, 214420 (2011).
  16. T. Gruner, J. Wykhoff, J. Sichelschmidt, C. Krellner, C. Geibel, and F. Steglich, Anisotropic electron spin resonance of YbIr2Si2, J. Phys.: Condens. Matter 22, 135602 (2010).
  17. S. Kabré, M. Julien Pouzol, and M. Guittard, Étude cristallographique des combinaisons ternaires formées par le thallium, les terres rares et le soufre, le sélénium ou le tellure, le long des binaires TL2X−L2X3, Bull. Soc. Chim. Fr. 9-10, 1881 (1974).
  18. M. Duczmal and L. Pawlak, Magnetic and structural characterization of TlLnSe2 compounds (Ln: Nd to Yb), J. Alloys Compd. 225, 181 (1995).
  19. A. Szczerbakow and K. Durose, Self-selecting vapour growth of bulk crystals – Principles and applicability, Prog. Cryst. Growth Charact. Mater. 51, 81 (2005).
  20. J.-Q. Yan and M. A. McGuire, Self-selecting vapor growth of transition-metal-halide single crystals, Phys. Rev. Mater. 7, 013401 (2023).
  21. A. A. Coelho, Topas and topas-academic: An optimization program integrating computer algebra and crystallographic objects written in C++, J. Appl. Crystallogr. 51, 210 (2018).
  22. A. A. Coelho, TOPAS Academic V4.1 Technical Reference (unpublished).
  23. Bruker, APEX Suite V.## (Bruker AXS Inc., Madison, WI, 2016).
  24. G. M. Sheldrick, A short history of SHELXL, Acta Crystallogr. Sect. A 64, 112 (2008).
  25. G. M. Sheldrick, Crystal structure refinement with SHELXL, Acta Crystallogr. C 71, 3 (2015).
  26. Y. Li, G. Chen, W. Tong, L. Pi, J. Liu, Z. Yang, X. Wang, and Q. Zhang, Rare-earth triangular lattice spin liquid: A single-crystal study of YbMgGaO4, Phys. Rev. Lett. 115, 167203 (2015).
  27. J. Sichelschmidt, P. Schlender, B. Schmidt, M. Baenitz, and T. Doert, Electron spin resonance on the spin-1/2 triangular magnet NaYbS2, J. Phys.: Condens. Matter 31, 205601 (2019).
  28. J. Sichelschmidt, B. Schmidt, P. Schlender, S. Khim, T. Doert, and M. Baenitz, Effective spin-1/2 moments on a Yb3+ triangular lattice: An ESR study, JPS Conf. Proc. 30, 011096 (2020).
  29. F. Grußler, M. Hemmida, S. Bachus, Y. Skourski, H.-A. Krug von Nidda, P. Gegenwart, and A. A. Tsirlin, Role of alkaline metal in the rare-earth triangular antiferromagnet KYbO2, Phys. Rev. B 107, 224416 (2023).
  30. S. Luther, K. M. Ranjith, Th. Doert, J. Wosnitza, H. Kühne, and M. Baenitz, Anisotropic magnetism and spin fluctuations in the triangular-lattice spin-liquid candidate NaYbSe2: A single-crystal Na23 and Se77 NMR study, Phys. Rev. B 110, 214440 (2024).
  31. T. Förster, F. A. Garcia, T. Gruner, E. E. Kaul, B. Schmidt, C. Geibel, and J. Sichelschmidt, Spin fluctuations with two-dimensional xy behavior in a frustrated s=12 square-lattice ferromagnet, Phys. Rev. B 87, 180401(R) (2013).
  32. H. Benner and J. P. Boucher, Spin dynamics in the paramagnetic regime: NMR and EPR in two-dimensional magnets, in Physics and Chemistry of Materials with Low-Dimensional Structures, Vol. 9, edited by L. J. De Jongh (Kluwer, Dordrecht, 1990), Chap. Magnetic properties of layered transition metal compounds, pp. 323–378.
  33. R. Orbach and B. Bleaney, Spin-lattice relaxation in rare-earth salts field dependence of the two-phonon process, Proc. Roy. Phys. Soc. A 264, 485 (1961).
  34. A. Abragam and B. Bleaney, Electron Paramagnetic Resonance of Transition Ions (Clarendon Press, Oxford, 1970).
  35. B. Halperin and P. C. Hohenberg, Generalization of scaling laws to dynamical properties of a system near its critical point, Phys. Rev. Lett. 19, 700 (1967).
  36. Z. Zhang, J. Li, M. Xie, W. Zhuo, D. T. Adroja, P. J. Baker, T. G. Perring, A. Zhang, F. Jin, J. Ji, X. Wang, J. Ma, and Q. Zhang, Low-energy spin dynamics of the quantum spin liquid candidate NaYbSe2, Phys. Rev. B 106, 085115 (2022).
  37. G. Agbeworvi, W. Zaheer, J. D. D. Ponis, J. V. V. Handy, J. R. R. Ayala, J. L. L. Andrews, P. Schofield, C. Jaye, C. Weiland, D. A. A. Fischer, and S. Banerjee, Effect of stereochemically active electron lone pairs on magnetic ordering in trivanadates, Inorg. Chem. 62, 12965 (2023).
  38. M. Baenitz, Data related to the manuscript entitled TlYbSe2 as a new member of the J=1/2 triangular lattice Yb delafossite family: From spin liquid to field-induced magnetic order, Edmond (2025), https://doi.org/10.17617/3.NIGLVV.

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Phys. Rev. B 112, 024426– Published 18 July, 2025
  • Received 13 May 2025
  • Accepted 8 July 2025
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Open access publication funded by Max Planck Society.

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