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
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 print issues and online access
$209.00 per year
only $17.42 per issue
Rent or buy this article
Prices vary by article type
from$1.95
to$39.95
Prices may be subject to local taxes which are calculated during checkout





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
Kools, J. Exchange-biased spin-valves for magnetic storage. IEEE Trans. Magn. 32, 3165–3184 (1996).
He, X. et al. Robust isothermal electric control of exchange bias at room temperature. Nat. Mater. 9, 579–585 (2010).
Meiklejohn, W. H. & Bean, C. P. New magnetic anisotropy. Phys. Rev. 102, 1413–1414 (1956).
Ohldag, H. et al. Correlation between exchange bias and pinned interfacial spins. Phys. Rev. Lett. 91, 017203 (2003).
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).
Kiwi, M. Exchange bias theory. J. Magn. Magn. Mater. 234, 584–595 (2001).
Miltényi, P. et al. Diluted antiferromagnets in exchange bias: proof of the domain state model. Phys. Rev. Lett. 84, 4224–4227 (2000).
Ali, M. et al. Exchange bias using a spin glass. Nat. Mater. 6, 70–75 (2007).
Giri, S., Patra, M. & Majumdar, S. Exchange bias effect in alloys and compounds. J. Phys. Condens. Matter 23, 073201 (2011).
Barnsley, L. C., Gray, E. M. & Webb, C. J. Asymmetric reversal in aged high concentration CuMn alloy. J. Phys. Condens. Matter 25, 086003 (2013).
Hudl, M., Mathieu, R. & Nordblad, P. Tunable exchange bias in dilute magnetic alloys—chiral spin glasses. Sci. Rep. 6, 19964 (2016).
Fischer, K. H. & Hertz, J. A. Spin Glasses (Cambridge Studies in Magnetism Vol. 1, Cambridge Univ. Press, 1993).
Mydosh, J. A. Spin Glasses: An Experimental Introduction (CRC Press, 2013).
Nagata, S., Keesom, P. H. & Harrison, H. R. Low-dc-field susceptibility of CuMn spin glass. Phys. Rev. B 19, 1633–1638 (1979).
Binder, K. & Young, A. P. Spin glasses: experimental facts, theoretical concepts, and open questions. Rev. Mod. Phys. 58, 801–976 (1986).
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).
Parisi, G. Order parameter for spin glasses. Phys. Rev. Lett. 50, 1946–1948 (1983).
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).
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).
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).
Doi, N. & Tazuke, Y. Spin glass phases in 2H-FexNbS2. J. Phys. Soc. Jpn 60, 3980–3981 (1991).
Yamamura, Y. et al. Heat capacity and phase transition of FexNbS2 at low temperature. J. Alloys Compd. 383, 338–341 (2004).
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).
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).
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).
Little, A. et al. Three-state nematicity in the triangular lattice antiferromagnet Fe1/3NbS2. Nat. Mater. 19, 1062–1067 (2020).
Nogués, J. & Schuller, I. K. Exchange bias. J. Magn. Magn. Mater. 192, 203–232 (1999).
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).
Malozemoff, A. Random-field model of exchange anisotropy at rough ferromagnetic-antiferromagnetic interfaces. Phys. Rev. B 35, 3679–3682 (1987).
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).
Chillal, S. et al. Microscopic coexistence of antiferromagnetic and spin-glass states. Phys. Rev. B 87, 220403 (2013).
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).
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).
Young, A. P. (ed.) Spin Glasses and Random Fields (Directions in Condensed Matter Physics Vol. 12, World Scientific, 1998).
Fishman, S. & Aharony, A. Random field effects in disordered anisotropic antiferromagnets. J. Phys. C 12, L729 (1979).
Cardy, J. L. Random-field effects in site-disordered Ising antiferromagnets. Phys. Rev. B 29, 505–507 (1984).
Malozemoff, A. P. Mechanisms of exchange anisotropy. J. Appl. Phys. 63, 3874–3879 (1988).
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
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
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.
Rights and permissions
About this article
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
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41567-020-01123-w
This article is cited by
-
Precursor region with full phonon softening above the charge-density-wave phase transition in 2H-TaSe2
Nature Communications (2023)
-
Spintronics intelligent devices
Science China Physics, Mechanics & Astronomy (2023)
-
Exchange-biased topological transverse thermoelectric effects in a Kagome ferrimagnet
Nature Communications (2022)
-
Symmetry-aware recursive image similarity exploration for materials microscopy
npj Computational Materials (2021)
-
Disordered exchange is biased
Nature Physics (2021)