Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Magnetic field induced ordering in the spin-12 chiral chain compound [Cu(pym)(H2O)4]SiF6·H2O

Rebecca Scatena1, Alberto Hernández-Melián2, Benjamin M. Huddart2,3, Sam Curley4, Robert C. Williams4, Pascal Manuel5, Stephen J. Blundell3, Zurab Guguchia6, Zachary E. Manson7 et al.

Jamie L. Manson7,*, G. Timothy Noe, II8, John Singleton8, Tom Lancaster2, Paul A. Goddard4,†, and Roger D. Johnson9,10

  • *Deceased.
  • †Contact author: p.goddard@warwick.ac.uk

Phys. Rev. B 112, 054414 – Published 5 August, 2025

DOI: https://doi.org/10.1103/w195-6pjw

Abstract

We present single-crystal neutron diffraction, powder muon spin rotation, and pulsed-field magnetometry measurements on the Heisenberg quantum chiral chain [Cu(pym)(H2O)4]SiF6·H2O (pym = pyrimidine), which displays a fourfold-periodic rotation of the local environment around the Cu(ii) S=1/2 ions from site to site along the chain. Previous measurements on this material have shown the absence of magnetic order down to surprisingly low temperatures ≥20 mK, as well as the presence of an energy gap for magnetic excitations that grows linearly with magnetic field. Here we find evidence at dilution refrigerator temperatures for a field-induced transition to long-range magnetic order above an applied magnetic field of 3 T. From the polarization of magnetic moments observed with magnetic fields applied in the [−1,2,0] direction, we can identify the static magnetic structure that best accounts for the data. The proposed model is supported microscopically by the presence of an alternating component of the g tensor, which produces an internal twofold staggered field that dictates both the direction of the ordered moments and the effective coupling between adjacent chains. The observed magnetic structure is contrary to previous proposals for the departure of the magnitude and field dependence of the energy gap from the predictions of the sine-Gordon model.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (25)

  1. D. C. Dender, P. R. Hammar, D. H. Reich, C. Broholm, and G. Aeppli, Direct observation of field-induced incommensurate fluctuations in a one-dimensional S=1/2 antiferromagnet, Phys. Rev. Lett. 79, 1750 (1997).
  2. M. Oshikawa and I. Affleck, Field-induced gap in S=1/2 antiferromagnetic chains, Phys. Rev. Lett. 79, 2883 (1997).
  3. I. Affleck and M. Oshikawa, Field-induced gap in Cu benzoate and other S=1/2 antiferromagnetic chains, Phys. Rev. B 60, 1038 (1999).
  4. R. Feyerherm, S. Abens, D. Günther, T. Ishida, M. Meißner, M. Meschke, T. Nogami, and M. Steiner, Magnetic-field induced gap and staggered susceptibility in the S=1/2 chain [PM·Cu(NO3)2·(H2O)2]n (PM = pyrimidine), J. Phys.: Condens. Matter 12, 8495 (2000).
  5. R. Helfrich, M. Köppen, M. Lang, F. Steglich, and A. Ochiai, New observations concerning the low-temperature properties of the carrier-poor heavy-fermion system Yb4As3, J. Magn. Magn. Mater. 177–181, 309 (1998).
  6. Y. Chen, M. B. Stone, M. Kenzelmann, C. D. Batista, D. H. Reich, and C. Broholm, Phase diagram and spin Hamiltonian of weakly-coupled anisotropic S=12 chains in CuCl2·2((CD3)2SO), Phys. Rev. B 75, 214409 (2007).
  7. F. H. L. Essler and A. M. Tsvelik, Dynamical magnetic susceptibilities in copper benzoate, Phys. Rev. B 57, 10592 (1998).
  8. F. H. L. Essler, A. Furusaki, and T. Hikihara, Dynamical structure factor in copper benzoate and other spin-1/2 antiferromagnetic chains, Phys. Rev. B 68, 064410 (2003).
  9. T. Asano, H. Nojiri, Y. Inagaki, J. P. Boucher, T. Sakon, Y. Ajiro, and M. Motokawa, ESR investigation on the breather mode and the spinon-breather dynamical crossover in Cu benzoate, Phys. Rev. Lett. 84, 5880 (2000).
  10. M. Kenzelmann, Y. Chen, C. Broholm, D. H. Reich, and Y. Qiu, Bound spinons in an antiferromagnetic S=1/2 chain with a staggered field, Phys. Rev. Lett. 93, 017204 (2004).
  11. S. A. Zvyagin, A. K. Kolezhuk, J. Krzystek, and R. Feyerherm, Excitation hierarchy of the quantum sine-Gordon spin chain in a strong magnetic field, Phys. Rev. Lett. 93, 027201 (2004).
  12. D. B. Cordes, C. V. Krishnamohan Sharma, and R. D. Rogers, Enantiomorphic helical coordination polymers of { [M(pyrimidine)(OH2)4][SiF6]·H2O}∞ (M = Co2+, Cu2+, Zn2+), Cryst. Growth Des. 7, 1943 (2007).
  13. J. Liu, S. Kittaka, R. D. Johnson, T. Lancaster, J. Singleton, T. Sakakibara, Y. Kohama, J. van Tol, A. Ardavan, B. H. Williams, S. J. Blundell, Z. E. Manson, J. L. Manson, and P. A. Goddard, Unconventional field-induced spin gap in an S=1/2 chiral staggered chain, Phys. Rev. Lett. 122, 057207 (2019).
  14. S. C. Furuya, Field-induced dimer orders in quantum spin chains, Phys. Rev. B 101, 134425 (2020).
  15. C. Yasuda, S. Todo, K. Hukushima, F. Alet, M. Keller, M. Troyer, and H. Takayama, Néel temperature of quasi-low-dimensional Heisenberg antiferromagnets, Phys. Rev. Lett. 94, 217201 (2005).
  16. W. Jin and O. A. Starykh, Phase diagram of weakly coupled Heisenberg spin chains subject to a uniform Dzyaloshinskii-Moriya interaction, Phys. Rev. B 95, 214404 (2017).
  17. L. C. Chapon, P. Manuel, P. G. Radaelli, C. Benson, L. Perrott, S. Ansell, N. J. Rhodes, D. Raspino, D. Duxbury, E. Spill, and J. Norris, Wish: The new powder and single crystal magnetic diffractometer on the second target station, Neutron News 22, 22 (2011).
  18. See Supplemental Material at http://link.aps.org/supplemental/10.1103/w195-6pjw for experimental details and a discussion of the calculations used in the μ+SR analysis.
  19. H. J. Schulz, Dynamics of coupled quantum spin chains, Phys. Rev. Lett. 77, 2790 (1996).
  20. T. Lancaster, S. J. Blundell, M. L. Brooks, P. J. Baker, F. L. Pratt, J. L. Manson, C. P. Landee, and C. Baines, Magnetic order in the quasi-one-dimensional spin-1/2 molecular chain compound copper pyrazine dinitrate, Phys. Rev. B 73, 020410(R) (2006).
  21. S. J. Blundell, R. De Renzi, T. Lancaster, and F. L. Pratt, Muon Spectroscopy: An Introduction (Oxford University Press, Oxford, 2022), p. 432.
  22. T. Lancaster, F. Xiao, B. M. Huddart, R. C. Williams, F. L. Pratt, S. J. Blundell, S. J. Clark, R. Scheuermann, T. Goko, S. Ward, J. L. Manson, C. Rüegg, and K. W. Krämer, Quantum magnetism in molecular spin ladders probed with muon-spin spectroscopy, New J. Phys. 20, 103002 (2018).
  23. A. L. Blockmon, M. Lee, S. Zhang, Z. E. Manson, J. L. Manson, V. S. Zapf, and J. L. Musfeldt, High field electrical polarization and magnetoelectric coupling in chiral magnet [Cu(pym)(H2O)4]SiF6·H2O, Inorg. Chem. 63, 11737 (2024).
  24. https://wrap.warwick.ac.uk/192071/.
  25. P. Goddard et al., An S = 1/2 chiral staggered chain in a magnetic field, STFC ISIS Neutron and Muon Source, 2019, https://doi.org/10.5286/ISIS.E.RB1910030.

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation