Spin liquid and ferroelectricity close to a quantum critical point in PbCuTe2O6
Source abstract
Abstract
Abstract Geometrical frustration among interacting spins combined with strong quantum fluctuations destabilize long-range magnetic order in favor of more exotic states such as spin liquids. By following this guiding principle, a number of spin liquid candidate systems were identified in quasi-two-dimensional (quasi-2D) systems. For 3D, however, the situation is less favorable as quantum fluctuations are reduced and competing states become more relevant. Here we report a comprehensive study of thermodynamic, magnetic and dielectric properties on single crystalline and pressed-powder samples of PbCuTe2O6, a candidate material for a 3D frustrated quantum spin liquid featuring a hyperkagome lattice. Whereas the low-temperature properties of the powder samples are consistent with the recently proposed quantum spin liquid state, an even more exotic behavior is revealed for the single crystals. These crystals show ferroelectric order at TFE ≈ 1 K, accompanied by strong lattice distortions, and a modified magnetic response—still consistent with a quantum spin liquid—but with clear indications for quantum critical behavior.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Advanced Condensed Matter Physics · Multiferroics and related materials · Algebraic structures and combinatorial models
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (44)
Show source-provided references
1. Balents, L. Spin liquids in frustrated magnets. Nature 464, 199–208 (2010).10.1038/nature08917 ↗
2. Lacroix, C., Mendels, P. & Mila, F. Introduction to Frustrated Magnetism. Springer Series in Solid-State Sciences Vol. 164 (Springer, New York, 2011).10.1007/978-3-642-10589-0 ↗
3. Savary, L. & Balents, L. Quantum spin liquids: a review. Rep. Prog. Phys. 80, 016502 (2017).10.1088/0034-4885/80/1/016502 ↗
4. Zhou, Y., Kanoda, K. & Ng, T.-K. Quantum spin liquid states. Rev. Mod. Phys. 89, 025003 (2017).10.1103/RevModPhys.89.025003 ↗
5. Broholm, C. et al. Quantum spin liquids. Science 367, eaay0668 (2020).10.1126/science.aay0668 ↗
6. Helton, J. S. et al. Spin dynamics of the spin-1/2 Kagome lattice antiferromagnet ZnCu3(OH)6Cl2. Phys. Rev. Lett. 98, 107204 (2007).10.1103/PhysRevLett.98.107204 ↗
7. Han, T.-H. et al. Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet. Nature 492, 406–410 (2012).10.1038/nature11659 ↗
8. Shimizu, Y. et al. Spin liquid state in an organic Mott insulator with a triangular lattice. Phys. Rev. Lett. 91, 107001 (2003).10.1103/PhysRevLett.91.107001 ↗
9. Itou, T. et al. Quantum spin liquid in the spin-1∕2 triangular antiferromagnet EtMe3Sb[Pd(dmit)2]2. Phys. Rev. B 77, 104413 (2008).10.1103/PhysRevB.77.104413 ↗
10. Powell, B. J. & McKenzie, R. H. Quantum frustration in organic Mott insulators: from spin liquids to unconventional superconductors. Rep. Prog. Phys. 74, 056501 (2011).10.1088/0034-4885/74/5/056501 ↗
11. Gardner, J. S., Gingras, M. J. P. & Greedan, J. E. Magnetic pyrochlore oxides. Rev. Mod. Phys. 82, 53 (2010).10.1103/RevModPhys.82.53 ↗
12. Rau, J. G. & Gingras, M. J. P. Frustrated quantum rare-earth pyrochlores. Annu. Rev. Condens. Matter Phys. 10, 357–386 (2019).10.1146/annurev-conmatphys-022317-110520 ↗
13. Okamoto, Y., Nohara, M., Aruga-Katori, H. & Takagi, H. Spin-liquid state in the S = 1/2 hyperkagome antiferromagnet Na4Ir3O8. Phys. Rev. Lett. 99, 137207 (2007).10.1103/PhysRevLett.99.137207 ↗
14. Elhajal, M., Canals, B. & Lacroix, C. Symmetry breaking due to Dzyaloshinsky-Moriya interactions in the kagome lattice. Phys. Rev. B 66, 014422 (2002).10.1103/PhysRevB.66.014422 ↗
15. Cépas, O., Fong, C. M., Leung, P. W. & Lhuillier, C. Quantum phase transition induced by Dzyaloshinskii-Moriya interactions in the kagome antiferromagnet. Phys. Rev. B 78, 140405(R) (2008).10.1103/PhysRevB.78.140405 ↗
16. Chen, G. & Balents, L. Spin-orbit effects in Na4Ir3O8: a hyper-kagome lattice antiferromagnet. Phys. Rev. B 78, 094403 (2008).10.1103/PhysRevB.78.094403 ↗
17. Singh, Y., Tokiwa, Y., Dong, J. & Gegenwart, P. Spin liquid close to a quantum critical point in Na4Ir3O8. Phys. Rev. B 88, 220413(R) (2013).10.1103/PhysRevB.88.220413 ↗
18. Koteswararao, B. et al. Magnetic properties and heat capacity of the three-dimensional frustrated S = 1/2 antiferromagnet PbCuTe2O6. Phys. Rev. B 90, 035141 (2014).10.1103/PhysRevB.90.035141 ↗
19. Khuntia, P. et al. Spin liquid state in the 3D frustrated antiferromagnet PbCuTe2O6: NMR and Muon spin relaxation studies. Phys. Rev. Lett. 116, 107203 (2016).10.1103/PhysRevLett.116.107203 ↗
20. Chillal, S. et al. Evidence for a three-dimensional quantum spin liquid in PbCuTe2O6. Nat. Commun. 11, 2348 (2020).10.1038/s41467-020-15594-1 ↗
21. Weil, M., Shirkhanlou, M. & Stürzer, T. Phase formation studies of lead(II) copper(II) oxotellurates: the crystal structures of dimorphic PbCuTeO5, PbCuTe2O6, and [Pb2Cu2(Te4O11)](NO3)2. Z. Anorg. Allg. Chem. 645, 347–353 (2019).10.1002/zaac.201800262 ↗
22. Koteswararao, B. et al. Observation of S = ½ quasi-1D magnetic and magneto-dielectric behavior in a cubic SrCuTe2O6. J. Phys.: Condens. Matter 27, 426001 (2015).
23. Hanna, A. R. N. et al. Crystal growth, characterization, and phase transition of PbCuTe2O6. Phys. Rev. Mater. 5, 113401 (2021).10.1103/PhysRevMaterials.5.113401 ↗
24. Köppen, M. et al. Solitary magnetic excitations in the low-carrier density, one-dimensional S = 1/2 antiferromagnet Yb4As3. Phys. Rev. Lett. 82, 4548–4551 (1999).10.1103/PhysRevLett.82.4548 ↗
25. Lines, M. E. & Glass, A. M. Principles and Application of Ferroelectrics and Related Materials (Clarendon Press, Oxford, 1977).
26. Lunkenheimer, P. et al. Multiferroicity in an organic charge-transfer salt that is suggestive of electric-dipole-driven magnetism. Nat. Mater. 11, 755–758 (2012).10.1038/nmat3400 ↗
27. Lu, J. et al. On the room temperature multiferroic BiFeO3: magnetic, dielectric and thermal properties. Eur. Phys. J. B 75, 451–460 (2010).10.1140/epjb/e2010-00170-x ↗
28. Wieder, H. H. Electrical behavior of barium titanate single crystals at low temperatures. Phys. Rev. 99, 1161–1165 (1955).10.1103/PhysRev.99.1161 ↗
29. Tokura, Y., Seki, S. & Nagaosa, N. Multiferroics of spin origin. Rep. Prog. Phys. 77, 076501 (2014).10.1088/0034-4885/77/7/076501 ↗
30. Zhong, W. L. et al. Phase transition in PbTiO3 ultrafine particles of different sizes. J. Phys.: Condens. Matter 5, 2619–2624 (1993).
31. Chattopadhyay, S., Ayyub, P., Palkar, V. R. & Multani, M. Size-induced diffuse phase transition in the nanocrystalline ferroelectric PbTiO3. Phys. Rev. B 52, 13177–13183 (1995).10.1103/PhysRevB.52.13177 ↗
32. Zhao, Z. et al. Grain-size effects on the ferroelectric behavior of dense nanocrystalline BaTiO3 ceramics. Phys. Rev. B 70, 024107 (2004).10.1103/PhysRevB.70.024107 ↗
33. Nakatsuji, S. et al. Spin disorder on a triangular lattice. Science 309, 1697–1700 (2005).10.1126/science.1114727 ↗
34. Cheng, J. G. et al. High-pressure sequence of Ba3NiSb2O9 structural phases: new S = 1 quantum spin liquids based on Ni2+. Phys. Rev. Lett. 107, 197204 (2011).10.1103/PhysRevLett.107.197204 ↗
35. Zhu, L., Garst, M., Rosch, A. & Si, Q. Universally diverging Grüneisen parameter and the magnetocaloric effect close to quantum critical points. Phys. Rev. Lett. 91, 066404 (2003).10.1103/PhysRevLett.91.066404 ↗
36. Tokiwa, Y. et al. Characteristic signatures of quantum criticality driven by geometrical frustration. Sci. Adv. e1500001 (2015).10.1126/sciadv.1500001 ↗
37. Tokiwa, Y., Ishikawa, J. J., Nakatsuji, S. & Gegenwart, P. Quantum criticality in a metallic spin liquid. Nat. Mater. 13, 356–359 (2014).10.1038/nmat3900 ↗
38. Matsumoto, Y. et al. Quantum criticality without tuning in the mixed valence compound β-YbAlB4. Science 331, 316–319 (2011).10.1126/science.1197531 ↗
39. Pott, R. & Schefzyk, R. Apparatus for measuring the thermal expansion of solids between 1.5 and 380 K. J. Phys. E 16, 444–449 (1983).10.1088/0022-3735/16/5/018 ↗
40. Fuller, G. H. Nuclear spins and moments. J. Phys. Chem. Ref. Data 5, 835–1092 (1976).10.1063/1.555544 ↗
41. De Bièvre, P. & Taylor, P. D. P. Table of the isotopic compositions of the elements. Int. J. Mass Spectrom. Ion-. Process. 123, 149–166 (1993).10.1016/0168-1176(93)87009-H ↗
42. Wolf, B. et al. Magnetocaloric effect and magnetic cooling near a field-induced quantum-critical point. Proc. Natl Acad. Sci. USA 108, 6862–6866 (2011).10.1073/pnas.1017047108 ↗
43. Kittel, Ch. Introduction to Solid State Physics (7th ed.) (John Wiley & Sons, Inc, New York, 1996).
44. Gati, E. et al. Evidence for electronically driven ferroelectricity in a strongly correlated dimerized BEDT-TTF molecular conductor. Phys. Rev. Lett. 120, 247601 (2018).10.1103/PhysRevLett.120.247601 ↗