- Physical Review Journals
All JournalsPhysics Magazine

Physical Review B

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

Short-range magnetic dynamics drive spin-phonon coupling above the Néel temperature in CrSBr

Zhe Zhang

Mustafa Mahmoud Aboulsaad

Ji Qi

Keda Jin and Felix Lüpke

Andreas Rydh

Roland Mathieu, Tomas Edvinsson, Zhaojun Li, and Peter Svedlindh*

  • Department of Materials Science and Engineering, Uppsala University, Box 35, SE-751 03 Uppsala, Sweden and WISE - Wallenberg Initiative Materials Science for Sustainability, Department of Materials Science and Engineering, Uppsala University, SE-751 03 Uppsala, Sweden

  • Department of Materials Science and Engineering, Uppsala University, Box 35, SE-751 03 Uppsala, Sweden

  • Department of Materials Science and Engineering, Uppsala University, Box 35, SE-751 03 Uppsala, Sweden

  • *Contact author: peter.svedlindh@angstrom.uu.se
PDF

Phys. Rev. B 114, 154426 – Published 25 September, 2026

DOI: https://doi.org/10.1103/pmln-p6vv

Abstract

Magnetic precursor temperature regimes in low-dimensional magnets provide a unique window into how spin, lattice, and electronic degrees of freedom become coupled before long-range spin order is established. Here we present a comprehensive investigation of the intertwined magnetic and lattice behavior above the Néel temperature (TN) in the van der Waals (vdW) antiferromagnet CrSBr. The results reveal a crossover from high-temperature two-dimensional (2D) XY behavior dominated by short-range ferromagnetic (FM) fluctuations to an intermediate three-dimensional (3D) state dominated by interlayer antiferromagnetic (AFM) correlations preceding the onset of long-range AFM order. The heat capacity shows only the anomaly associated with AFM ordering, further indicating that this intermediate regime does not correspond to an additional thermodynamic phase transition. Polarized Raman measurements reveal phonon self-energy anomalies and relative intensity changes above TN, indicating that the lattice dynamics have already renormalized in the magnetic precursor regime. These findings support the conclusion that dynamic spin-phonon coupling in CrSBr is already established prior to long-range AFM ordering and is mediated by short-range magnetic correlations.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (48)

  1. B. Huang, G. Clark, E. Navarro-Moratalla, D. R. Klein, R. Cheng, K. L. Seyler, D. Zhong, E. Schmidgall, M. A. McGuire, D. H. Cobden, et al., Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit, Nature (London) 546, 270 (2017).
  2. C. Gong, L. Li, Z. Li, H. Ji, A. Stern, Y. Xia, T. Cao, W. Bao, C. Wang, Y. Wang, et al., Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals, Nature (London) 546, 265 (2017).
  3. N. D. Mermin and H. Wagner, Absence of ferromagnetism or antiferromagnetism in one-or two-dimensional isotropic Heisenberg models, Phys. Rev. Lett. 17, 1133 (1966).
  4. P. C. Hohenberg, Existence of long-range order in one and two dimensions, Phys. Rev. 158, 383 (1967).
  5. S. Coleman, There are no Goldstone bosons in two dimensions, Commun. Math. Phys. 31, 259 (1973).
  6. P. Liu, Y. Zhang, K. Li, Y. Li, and Y. Pu, Recent advances in 2D van der Waals magnets: Detection, modulation, and applications, iScience 26, 107584 (2023).
  7. B. Zhang, P. Lu, R. Tabrizian, P. X.-L. Feng, and Y. Wu, 2D magnetic heterostructures: Spintronics and quantum future, npj Spintronics 2, 6 (2024).
  8. J. Dang, T. Wu, S. Yan, K. Watanabe, T. Taniguchi, H. Lei, and X.-X. Zhang, Electrical switching of spin-polarized light-emitting diodes based on a 2D CrI3/hBN/WSe2 heterostructure, Nat. Commun. 15, 6799 (2024).
  9. Z. Jia, M. Zhao, Q. Chen, Y. Tian, L. Liu, F. Zhang, D. Zhang, Y. Ji, B. Camargo, K. Ye, et al., Spintronic devices upon 2D magnetic materials and heterojunctions, ACS Nano 19, 9452 (2025).
  10. S. Liu, I. A. Malik, V. L. Zhang, and T. Yu, Lightning the spin: Harnessing the potential of 2D magnets in opto-spintronics, Adv. Mater. 37, 2306920 (2025).
  11. H. Yang, S. O. Valenzuela, M. Chshiev, S. Couet, B. Dieny, B. Dlubak, A. Fert, K. Garello, M. Jamet, D.-E. Jeong, et al., Two-dimensional materials prospects for non-volatile spintronic memories, Nature (London) 606, 663 (2022).
  12. D. Marković, A. Mizrahi, D. Querlioz, and J. Grollier, Physics for neuromorphic computing, Nat. Rev. Phys. 2, 499 (2020).
  13. E. J. Telford, A. H. Dismukes, R. L. Dudley, R. A. Wiscons, K. Lee, D. G. Chica, M. E. Ziebel, M.-G. Han, J. Yu, S. Shabani, et al., Coupling between magnetic order and charge transport in a two-dimensional magnetic semiconductor, Nat. Mater. 21, 754 (2022).
  14. N. P. Wilson, K. Lee, J. Cenker, K. Xie, A. H. Dismukes, E. J. Telford, J. Fonseca, S. Sivakumar, C. Dean, T. Cao, et al., Interlayer electronic coupling on demand in a 2D magnetic semiconductor, Nat. Mater. 20, 1657 (2021).
  15. F. Wu, I. Gutiérrez-Lezama, S. A. López-Paz, M. Gibertini, K. Watanabe, T. Taniguchi, F. O. von Rohr, N. Ubrig, and A. F. Morpurgo, Quasi-1D electronic transport in a 2D magnetic semiconductor, Adv. Mater. 34, 2109759 (2022).
  16. M. E. Ziebel, M. L. Feuer, J. Cox, X. Zhu, C. R. Dean, and X. Roy, CrSBr: An air-stable, two-dimensional magnetic semiconductor, Nano Lett. 24, 4319 (2024).
  17. T. M. J. Cham, S. Karimeddiny, A. H. Dismukes, X. Roy, D. C. Ralph, and Y. K. Luo, Anisotropic gigahertz antiferromagnetic resonances of the easy-axis van der Waals antiferromagnet CrSBr, Nano Lett. 22, 6716 (2022).
  18. F. Long, K. Mosina, R. Hübner, Z. Sofer, J. Klein, S. Prucnal, M. Helm, F. Dirnberger, and S. Zhou, Intrinsic magnetic properties of the layered antiferromagnet CrSBr, Appl. Phys. Lett. 123, 222401 (2023).
  19. K. Lee, A. H. Dismukes, E. J. Telford, R. A. Wiscons, J. Wang, X. Xu, C. Nuckolls, C. R. Dean, X. Roy, and X. Zhu, Magnetic order and symmetry in the 2D semiconductor CrSBr, Nano Lett. 21, 3511 (2021).
  20. S. A. López-Paz, Z. Guguchia, V. Y. Pomjakushin, C. Witteveen, A. Cervellino, H. Luetkens, N. Casati, A. F. Morpurgo, and F. O. von Rohr, Dynamic magnetic crossover at the origin of the hidden-order in van der Waals antiferromagnet CrSBr, Nat. Commun. 13, 4745 (2022).
  21. S. T. Bramwell and P. C. W. Holdsworth, Magnetization and universal sub-critical behaviour in two-dimensional XY magnets, J. Phys.: Condens. Matter 5, L53 (1993).
  22. W. Liu, X. Guo, J. Schwartz, H. Xie, N. U. Dhale, S. H. Sung, A. L. N. Kondusamy, X. Wang, H. Zhao, D. Berman, R. Hovden, L. Zhao, and B. Lv, A three-stage magnetic phase transition revealed in ultrahigh-quality van der Waals bulk magnet CrSBr, ACS Nano 16, 15917 (2022).
  23. X. Guo, W. Liu, J. Schwartz, S. H. Sung, D. Zhang, M. Shimizu, A. L. N. Kondusamy, L. Li, K. Sun, H. Deng, H. O. Jeschke, I. I. Mazin, R. Hovden, B. Lv, and L. Zhao, Extraordinary phase transition revealed in a van der Waals antiferromagnet, Nat. Commun. 15, 6472 (2024).
  24. X. Wei, M. Li, X. He, Q. Xie, L. Chen, L. Ma, and G. Cheng, Spin–phonon coupling and phonon dynamics in van der Waals antiferromagnetic CrSBr, Appl. Phys. Lett. 126, 252201 (2025).
  25. A. Pawbake, T. Pelini, N. P. Wilson, K. Mosina, Z. Sofer, R. Heid, and C. Faugeras, Raman scattering signatures of strong spin-phonon coupling in the bulk magnetic van der Waals material CrSBr, Phys. Rev. B 107, 075421 (2023).
  26. A. Rybakov, C. Boix-Constant, D. Alba Venero, H. S. J. van der Zant, S. Mañas-Valero, and E. Coronado, Probing short-range correlations in the van der Waals magnet CrSBr by small-angle neutron scattering, Small Science 4, 2400244 (2024).
  27. G. Lan, H. Xu, Y. Zhang, C. Cheng, B. He, J. Li, C. He, C. Wan, J. Feng, H. Wei, et al., Giant tunneling magnetoresistance in spin-filter magnetic tunnel junctions based on van der Waals A-type antiferromagnet CrSBr, Chin. Phys. Lett. 40, 058501 (2023).
  28. S. Tagliati, V. M. Krasnov, and A. Rydh, Differential membrane-based nanocalorimeter for high-resolution measurements of low-temperature specific heat, Rev. Sci. Instrum. 83, 055107 (2012).
  29. G. Ramirez-Santiago and J. V. José, Critical exponents of the fully frustrated two-dimensional XY model, Phys. Rev. B 49, 9567 (1994).
  30. C. Boix-Constant, S. Mañas-Valero, A. M. Ruiz, A. Rybakov, K. A. Konieczny, S. Pillet, J. J. Baldoví, and E. Coronado, Probing the spin dimensionality in single-layer CrSBr van der Waals heterostructures by magneto-transport measurements, Adv. Mater. 34, 2204940 (2022).
  31. J. Klein, Z. Song, B. Pingault, F. Dirnberger, H. Chi, J. B. Curtis, R. Dana, R. Bushati, J. Quan, L. Dekanovsky, Z. Sofer, A. Alù, V. M. Menon, J. S. Moodera, M. Lončar, P. Narang, and F. M. Ross, Sensing the local magnetic environment through optically active defects in a layered magnetic semiconductor, ACS Nano 17, 288 (2023).
  32. E. J. Telford, A. H. Dismukes, K. Lee, M. Cheng, A. Wieteska, A. K. Bartholomew, Y.-S. Chen, X. Xu, A. N. Pasupathy, X. Zhu, C. R. Dean, and X. Roy, Layered antiferromagnetism induces large negative magnetoresistance in the van der Waals semiconductor CrSBr, Adv. Mater. 32, 2003240 (2020).
  33. L. Liu and J. T. C. Liu, Theory of the bound magnetic polaron in antiferromagnetic semiconductors, Phys. Rev. B 33, 1797 (1986).
  34. S. W. Song, J. Klein, K. Mosina, Z. Sofer, D. Sedmidubský, J. Dong, K. Chen, F. M. Ross, and R. Jaramillo, Magnetic secondary phases in the annealed van der Waals antiferromagnet CrSBr, J. Phys. Chem. C 129, 19002 (2025).
  35. See Supplemental Material at http://link.aps.org/supplemental/10.1103/pmln-p6vv for AFM spin arrangements and in-plane magnetic domains; in-phase component of the ac susceptibility; magnetization along different axes; out-of-phase component of the ac susceptibility; heat capacity, magnetic susceptibility under different fields; polarized Raman spectroscopy data.
  36. A. Bogdanov, A. Zhuravlev, and V. Telepa, The magnetic phase diagram of (C2H5NH3)2CuCl4, Sov. J. Low Temp. Phys. 10, 331 (1984).
  37. A. Bogdanov, A. Puzynya, V. Telepa, and P. Shatskiĩ, Influence of pressure on the magnetic (H-T) phase diagram of the rhombic antiferromagnet (C2H5NH3)2CuCl4, Sov. J. Low Temp. Phys. 13, 40 (1987).
  38. M. A. Tschudin, D. A. Broadway, P. Siegwolf, C. Schrader, E. J. Telford, B. Gross, J. Cox, A. E. E. Dubois, D. G. Chica, R. Rama-Eiroa, E. J. G. Santos, M. Poggio, M. E. Ziebel, C. R. Dean, X. Roy, and P. Maletinsky, Imaging nanomagnetism and magnetic phase transitions in atomically thin CrSBr, Nat. Commun. 15, 6005 (2024).
  39. L. De Jongh, W. Van Amstel, and A. Miedema, Magnetic measurements on (C2H5NH3)2CuCl4: Ferromagnetic layers coupled by a very weak antiferromagnetic interaction, Physica (Amsterdam) 58, 277 (1972).
  40. J. Shi, D. Wang, N. Jiang, Z. Xin, H. Zheng, C. Shen, X. Zhang, and X. Liu, Giant magneto-exciton coupling in 2D van der Waals CrSBr, ACS Nano 19, 29977 (2025).
  41. K. Lin, X. Sun, F. Dirnberger, Y. Li, J. Qu, P. Wen, Z. Sofer, A. Söll, S. Winnerl, M. Helm, S. Zhou, Y. Dan, and S. Prucnal, Strong exciton–phonon coupling as a fingerprint of magnetic ordering in van der Waals layered CrSBr, ACS Nano 18, 2898 (2024).
  42. Y. Zhai, Y. Tang, T. Zhou, H. Li, T. Qin, Z. Sofer, L. Hu, and Q. Xiong, Anisotropic magneto-optical Raman response coupled with magnetic ordering in an A-type antiferromagnet, Nano Lett. 25, 12570 (2025).
  43. P. Klemens, Anharmonic decay of optical phonons, Phys. Rev. 148, 845 (1966).
  44. Y. Tian, M. J. Gray, H. Ji, R. J. Cava, and K. S. Burch, Magneto-elastic coupling in a potential ferromagnetic 2D atomic crystal, 2D Mater. 3, 025035 (2016).
  45. C. J. Fennie and K. M. Rabe, Magnetically induced phonon anisotropy in ZnCr2O4 from first principles, Phys. Rev. Lett. 96, 205505 (2006).
  46. S. Djurdjić Mijin, A. Šolajić, J. Pešić, Y. Liu, C. Petrovic, M. Bockstedte, A. Bonanni, Z. V. Popović, and N. Lazarević, Spin-phonon interaction and short-range order in Mn3Si2Te6, Phys. Rev. B 107, 054309 (2023).
  47. J. Laverdière, S. Jandl, A. A. Mukhin, V. Y. Ivanov, V. G. Ivanov, and M. N. Iliev, Spin-phonon coupling in orthorhombic RMnO3 (R = Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Y): A Raman study, Phys. Rev. B 73, 214301 (2006).
  48. E. Granado, A. García, J. Sanjurjo, C. Rettori, I. Torriani, F. Prado, R. Sánchez, A. Caneiro, and S. Oseroff, Magnetic ordering effects in the Raman spectra of La1−xMn1−xO3, Phys. Rev. B 60, 11879 (1999).

Outline

Information

Phys. Rev. B 114, 154426– Published 25 September, 2026
  • Received 21 April 2026
  • Revised 13 August 2026
  • Accepted 31 August 2026
Crossmark - Check for updates button
Creative Commons Logo

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. Funded by Bibsam.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation