Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Exchange bias due to coupling between coexisting antiferromagnetic and spin-glass orders

Nature Physics volume 17, pages 525–530 (2021)Cite this article

Subjects

Abstract

Exchange bias is a property of widespread technological utility, but its underlying mechanism remains elusive, in part because it is rooted in the interaction of coexisting order parameters in the presence of complex magnetic disorder. Here we show that a giant exchange bias housed within a spin-glass phase arises in a disordered antiferromagnet. The magnitude and robustness of the exchange bias emerges from a convolution of two energetic landscapes, namely the highly degenerate landscape of the spin glass biased by the sublattice spin configuration of the antiferromagnet. The former provides a source of uncompensated moment, whereas the latter provides a mechanism for its pinning, which leads to the exchange bias. Tuning the relative strengths of the spin-glass and antiferromagnetic order parameters reveals a principle for tailoring the exchange bias, with potential applications to spintronic technologies.

This is a preview of subscription content, access via your institution

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Spin glass characterization of FexNbS2 for x = 0.30 and x = 0.35.
Fig. 2: Low-field exchange bias characterization.
Fig. 3: Temperature and field sweep dependencies of the exchange bias and coercive fields.
Fig. 4: NMR measurements performed on x = 0.30, 0.33 and 0.35 intercalations.
Fig. 5: High-field exchange bias characterization.

Similar content being viewed by others

Data availability

Source data are provided with this paper. All other data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.

References

  1. Kools, J. Exchange-biased spin-valves for magnetic storage. IEEE Trans. Magn. 32, 3165–3184 (1996).

    Article  ADS  Google Scholar 

  2. He, X. et al. Robust isothermal electric control of exchange bias at room temperature. Nat. Mater. 9, 579–585 (2010).

    Article  ADS  Google Scholar 

  3. Meiklejohn, W. H. & Bean, C. P. New magnetic anisotropy. Phys. Rev. 102, 1413–1414 (1956).

    Article  ADS  Google Scholar 

  4. Ohldag, H. et al. Correlation between exchange bias and pinned interfacial spins. Phys. Rev. Lett. 91, 017203 (2003).

    Article  ADS  Google Scholar 

  5. Schuller, I. K., Morales, R., Batlle, X., Nowak, U. & Güntherodt, G. Role of the antiferromagnetic bulk spins in exchange bias. J. Magn. Magn. Mater. 416, 2–9 (2016).

    Article  ADS  Google Scholar 

  6. Kiwi, M. Exchange bias theory. J. Magn. Magn. Mater. 234, 584–595 (2001).

    Article  ADS  Google Scholar 

  7. Miltényi, P. et al. Diluted antiferromagnets in exchange bias: proof of the domain state model. Phys. Rev. Lett. 84, 4224–4227 (2000).

    Article  ADS  Google Scholar 

  8. Ali, M. et al. Exchange bias using a spin glass. Nat. Mater. 6, 70–75 (2007).

    Article  ADS  Google Scholar 

  9. Giri, S., Patra, M. & Majumdar, S. Exchange bias effect in alloys and compounds. J. Phys. Condens. Matter 23, 073201 (2011).

    Article  ADS  Google Scholar 

  10. Barnsley, L. C., Gray, E. M. & Webb, C. J. Asymmetric reversal in aged high concentration CuMn alloy. J. Phys. Condens. Matter 25, 086003 (2013).

    Article  ADS  Google Scholar 

  11. Hudl, M., Mathieu, R. & Nordblad, P. Tunable exchange bias in dilute magnetic alloys—chiral spin glasses. Sci. Rep. 6, 19964 (2016).

    Article  ADS  Google Scholar 

  12. Fischer, K. H. & Hertz, J. A. Spin Glasses (Cambridge Studies in Magnetism Vol. 1, Cambridge Univ. Press, 1993).

  13. Mydosh, J. A. Spin Glasses: An Experimental Introduction (CRC Press, 2013).

  14. Nagata, S., Keesom, P. H. & Harrison, H. R. Low-dc-field susceptibility of CuMn spin glass. Phys. Rev. B 19, 1633–1638 (1979).

    Article  ADS  Google Scholar 

  15. Binder, K. & Young, A. P. Spin glasses: experimental facts, theoretical concepts, and open questions. Rev. Mod. Phys. 58, 801–976 (1986).

    Article  ADS  Google Scholar 

  16. Dekker, C., Arts, A. F., de Wijn, H. W., van Duyneveldt, A. J. & Mydosh, J. A. Activated dynamics in a two-dimensional Ising spin glass: Rb2Cu1−xCoxF4. Phys. Rev. B 40, 11243–11251 (1989).

    Article  ADS  Google Scholar 

  17. Parisi, G. Order parameter for spin glasses. Phys. Rev. Lett. 50, 1946–1948 (1983).

    Article  ADS  MathSciNet  Google Scholar 

  18. Van Laar, B., Rietveld, H. M. & Ijdo, D. J. W. Magnetic and crystallographic structures of MexNbS2 and MexTaS2. J. Solid State Chem. 3, 154–160 (1971).

    Article  ADS  Google Scholar 

  19. Suzuki, T., Ikeda, S., Richardson, J. W. & Yamaguchi, Y. Magnetic structure of Fe1/3NbS2. In Proc. 5th International Symposium on Advanced Nuclear Energy Research 343–346 (Japan Atomic Energy Research Institute, 1993).

  20. Haley, S. C. et al. Half-magnetization plateau and the origin of threefold symmetry breaking in an electrically switchable triangular antiferromagnet. Phys. Rev. Res. 2, 043020 (2020).

    Article  Google Scholar 

  21. Doi, N. & Tazuke, Y. Spin glass phases in 2H-FexNbS2. J. Phys. Soc. Jpn 60, 3980–3981 (1991).

    Article  ADS  Google Scholar 

  22. Yamamura, Y. et al. Heat capacity and phase transition of FexNbS2 at low temperature. J. Alloys Compd. 383, 338–341 (2004).

    Article  Google Scholar 

  23. Tsuji, T., Yamamura, Y., Watanabe, H., Saito, K. & Sorai, M. Heat capacity of intercalated layered materials FexNbS2 at low temperature. J. Therm. Anal. Calorim. 57, 839–846 (1999).

    Article  Google Scholar 

  24. Parkin, S. S. P. & Friend, R. H. 3d transition-metal intercalates of the niobium and tantalum dichalcogenides. II. Transport properties. Phil. Mag. B 41, 95–112 (1980).

    Article  ADS  Google Scholar 

  25. Friend, R. H., Beal, A. R. & Yoffe, A. D. Electrical and magnetic properties of some first row transition metal intercalates of niobium disulphide. Phil. Mag. 35, 1269–1287 (1977).

    Article  ADS  Google Scholar 

  26. Little, A. et al. Three-state nematicity in the triangular lattice antiferromagnet Fe1/3NbS2. Nat. Mater. 19, 1062–1067 (2020).

    Article  ADS  Google Scholar 

  27. Nogués, J. & Schuller, I. K. Exchange bias. J. Magn. Magn. Mater. 192, 203–232 (1999).

    Article  ADS  Google Scholar 

  28. Büttgen, N., Kuhns, P., Prokofiev, A., Reyes, A. P. & Svistov, L. E. High-field NMR of the quasi-one-dimensional antiferromagnet LiCuVO4. Phys. Rev. B 85, 214421 (2012).

    Article  ADS  Google Scholar 

  29. Malozemoff, A. Random-field model of exchange anisotropy at rough ferromagnetic-antiferromagnetic interfaces. Phys. Rev. B 35, 3679–3682 (1987).

    Article  ADS  Google Scholar 

  30. Wong, P. et al. Coexistence of spin-glass and antiferromagnetic orders in the Ising system Fe0.55Mg0.45Cl2. Phys. Rev. Lett. 55, 2043–2046 (1985).

    Article  ADS  Google Scholar 

  31. Chillal, S. et al. Microscopic coexistence of antiferromagnetic and spin-glass states. Phys. Rev. B 87, 220403 (2013).

    Article  ADS  Google Scholar 

  32. Kleemann, W., Shvartsman, V. V., Borisov, P. & Kania, A. Coexistence of antiferromagnetic and spin cluster glass order in the magnetoelectric relaxor multiferroic PbFe0.5Nb0.5O3. Phys. Rev. Lett. 105, 257202 (2010).

    Article  ADS  Google Scholar 

  33. Fu, Z. et al. Coexistence of magnetic order and spin-glass-like phase in the pyrochlore antiferromagnet Na3Co(Co3)2Cl. Phys. Rev. B 87, 214406 (2013).

    Article  ADS  Google Scholar 

  34. Young, A. P. (ed.) Spin Glasses and Random Fields (Directions in Condensed Matter Physics Vol. 12, World Scientific, 1998).

  35. Fishman, S. & Aharony, A. Random field effects in disordered anisotropic antiferromagnets. J. Phys. C 12, L729 (1979).

    Article  ADS  Google Scholar 

  36. Cardy, J. L. Random-field effects in site-disordered Ising antiferromagnets. Phys. Rev. B 29, 505–507 (1984).

    Article  ADS  Google Scholar 

  37. Malozemoff, A. P. Mechanisms of exchange anisotropy. J. Appl. Phys. 63, 3874–3879 (1988).

    Article  ADS  Google Scholar 

Download references

Acknowledgements

This work was supported as part of the Center for Novel Pathways to Quantum Coherence in Materials, an Energy Frontier Research Center funded by the United States Department of Energy, Office of Science, Basic Energy Sciences. Work by J.G.A. was partially supported by the EPiQS Initiative of the Gordon and Betty Moore Foundation through grant no. GBMF9067. R.A.M. and J.R.L. were supported by the National Science Foundation through award no. DMR-1611525. A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by the National Science Foundation cooperative agreement no. DMR-1644779 and the State of Florida. Laue microdiffraction measurements were done with the assistance of C. Stan in the Advanced Light Source beamline 12.3.2, which is an Office of Science User Facility of the Department of Energy, under contract no. DE-AC02-05CH11231.

Author information

Authors and Affiliations

  1. Department of Physics, University of California, Berkeley, CA, USA

    Eran Maniv, Shannon C. Haley, Spencer Doyle, Caolan John, Yun-Long Tang, Ramamoorthy Ramesh & James G. Analytis

  2. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Eran Maniv, Shannon C. Haley, Spencer Doyle, Caolan John, Yun-Long Tang, Ramamoorthy Ramesh, Jeffrey R. Long & James G. Analytis

  3. Department of Chemistry, University of California, Berkeley, CA, USA

    Ryan A. Murphy & Jeffrey R. Long

  4. Nuclear Research Center – Negev, Beer Sheva, Israel

    Ariel Maniv

  5. National High Magnetic Field Laboratory, Tallahassee, FL, USA

    Ariel Maniv, Sanath K. Ramakrishna & Arneil P. Reyes

  6. Department of Materials Science and Engineering, University of California, Berkeley, CA, USA

    Yun-Long Tang & Ramamoorthy Ramesh

  7. National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Peter Ercius

  8. Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA, USA

    Jeffrey R. Long

Authors
  1. Eran Maniv
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Ryan A. Murphy
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Shannon C. Haley
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Spencer Doyle
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Caolan John
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Ariel Maniv
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Sanath K. Ramakrishna
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Yun-Long Tang
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Peter Ercius
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Ramamoorthy Ramesh
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Arneil P. Reyes
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Jeffrey R. Long
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. James G. Analytis
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

E.M., S.D., C.J. and S.C.H. performed crystal synthesis and magnetization measurements. E.M. performed heat capacity, energy-dispersive X-ray spectroscopy and Laue microdiffraction measurements. R.A.M. and J.R.L. assisted in initial measurements and interpretation of glassy behaviour and exchange bias, and performed inductively coupled plasma analysis. A.M., S.K.R. and A.P.R. performed NMR measurements. Y.-L.T., P.E. and R.R. performed transmission electron microscopy measurements and analysis. E.M., R.A.M. and J.G.A. performed data analysis and wrote the manuscript with input from all co-authors.

Corresponding authors

Correspondence to Eran Maniv or James G. Analytis.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Peer review information Nature Physics thanks Per Nordblad and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Figs. 1–18, Sections 1–15 and Tables 1–3.

Supplementary Video 1

Laue microdiffraction measurements showing the diffraction peaks combined with the 2H-Fe1/3NbS2 structure fits (the squares on top). The attached movie presents a homogeneous structure along approximately 35 μm lateral scan for x = 0.30 intercalation. The scan range was determined by the size of the sample.

Supplementary Video 2

Laue microdiffraction measurements showing the diffraction peaks combined with the 2H-Fe1/3NbS2 structure fits (the squares on top). The attached movies present a homogeneous structure along approximately 350 μm lateral scan for x = 0.31 intercalation. The scan range was determined by the size of the sample.

Source data

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Maniv, E., Murphy, R.A., Haley, S.C. et al. Exchange bias due to coupling between coexisting antiferromagnetic and spin-glass orders. Nat. Phys. 17, 525–530 (2021). https://doi.org/10.1038/s41567-020-01123-w

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41567-020-01123-w

This article is cited by

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing