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Configurable antiferromagnetic domains and lateral exchange bias in atomically thin CrPS4

Nature Materials volume 24, pages 1414–1423 (2025)Cite this article

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Abstract

Interfacial exchange coupling between antiferromagnets (AFMs) and ferromagnets (FMs) crucially makes it possible to shift the FM hysteresis, known as exchange bias, and to switch AFM states. Two-dimensional magnets unlock opportunities to combine AFM and FM materials; however, the buried AFM–FM interfaces obtained by stacking remains challenging to understand. Here we demonstrate interfacial control via intralayer exchange coupling in the layered AFM CrPS4, where connected even and odd layers realize pristine lateral interfaces between AFM-like and FM-like regions. We distinguish antiphase even-layer states by scanning nitrogen-vacancy centre magnetometry due to a weak surface magnetization. This surface magnetization enables control over the even-layer state, with different regions switching at distinct fields due to their own lateral couplings. We toggle three AFM domains adjacent to a FM-like region and demonstrate a tunable multilevel exchange bias. Our nanoscale visualization unveils the microscopic origins of exchange bias and advances single two-dimensional crystals for hybrid AFM–FM technologies.

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Fig. 1: Layered AFM in atomically thin CrPS4.
Fig. 2: Antiphase domains in even-layer CrPS4.
Fig. 3: Lateral exchange bias at the even–odd interface.
Fig. 4: Controlled nucleation and translation of AFM domain walls.
Fig. 5: Multilevel exchange bias through digital control of AFM domains.

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All data that support the findings of this study are available from the corresponding author upon request. Source data are provided with this paper.

Code availability

The codes that support the findings of this study are available upon request. Codes include scripts for data analysis and micromagnetic simulations.

References

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

    Article  Google Scholar 

  2. Song, C. et al. How to manipulate magnetic states of antiferromagnets. Nanotechnology 29, 112001 (2018).

    Article  PubMed  Google Scholar 

  3. Fukami, S., Zhang, C., DuttaGupta, S., Kurenkov, A. & Ohno, H. Magnetization switching by spin–orbit torque in an antiferromagnet–ferromagnet bilayer system. Nat. Mater. 15, 535–541 (2016).

    Article  CAS  PubMed  Google Scholar 

  4. Peng, S. et al. Exchange bias switching in an antiferromagnet/ferromagnet bilayer driven by spin–orbit torque. Nat. Electron. 3, 757–764 (2020).

    Article  CAS  Google Scholar 

  5. Kang, J. et al. Current-induced manipulation of exchange bias in IrMn/NiFe bilayer structures. Nat. Commun. 12, 6420 (2021).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  6. Nayak, A. K. et al. Design of compensated ferrimagnetic Heusler alloys for giant tunable exchange bias. Nat. Mater. 14, 679–684 (2015).

    Article  CAS  PubMed  Google Scholar 

  7. Maniv, E. et al. Exchange bias due to coupling between coexisting antiferromagnetic and spin-glass orders. Nat. Phys. 17, 525–530 (2021).

    Article  CAS  Google Scholar 

  8. Stiles, M. D. & McMichael, R. D. Model for exchange bias in polycrystalline ferromagnet–antiferromagnet bilayers. Phys. Rev. B 59, 3722–3733 (1999).

    Article  CAS  Google Scholar 

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

    Article  PubMed  Google Scholar 

  10. Scholl, A., Liberati, M., Arenholz, E., Ohldag, H. & Stöhr, J. Creation of an antiferromagnetic exchange spring. Phys. Rev. Lett. 92, 247201 (2004).

    Article  CAS  PubMed  Google Scholar 

  11. Park, B. G. et al. A spin-valve-like magnetoresistance of an antiferromagnet-based tunnel junction. Nat. Mater. 10, 347–351 (2011).

    Article  CAS  PubMed  Google Scholar 

  12. Noah, A. et al. Tunable exchange bias in the magnetic Weyl semimetal Co3Sn2S2. Phys. Rev. B 105, 144423 (2022).

    Article  CAS  Google Scholar 

  13. Zheng, G. et al. Gate-tuned interlayer coupling in van der Waals ferromagnet Fe3GeTe2 nanoflakes. Phys. Rev. Lett. 125, 047202 (2020).

    Article  CAS  PubMed  Google Scholar 

  14. Gweon, H. K. et al. Exchange bias in weakly interlayer-coupled van der Waals magnet Fe3GeTe2. Nano Lett. 21, 1672–1678 (2021).

    Article  CAS  PubMed  Google Scholar 

  15. Chong, S. K. et al. Intrinsic exchange biased anomalous Hall effect in an uncompensated antiferromagnet MnBi2Te4. Nat. Commun. 15, 2881 (2024).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  16. Chen, B. et al. Even-odd layer-dependent exchange bias effect in MnBi2Te4 Chern insulator devices. Nano Lett. 24, 8320–8326 (2024).

    Article  CAS  PubMed  Google Scholar 

  17. Zhu, R. et al. Exchange bias in van der Waals CrCl3/Fe3GeTe2 heterostructures. Nano Lett. 20, 5030–5035 (2020).

    Article  CAS  PubMed  Google Scholar 

  18. Albarakati, S. et al. Electric control of exchange bias effect in FePS3–Fe5GeTe2 van der Waals heterostructures. Nano Lett. 22, 6166–6172 (2022).

    Article  CAS  PubMed  Google Scholar 

  19. Ying, Z. et al. Large exchange bias effect and coverage-dependent interfacial coupling in CrI3/MnBi2Te4 van der Waals heterostructures. Nano Lett. 23, 765–771 (2023).

    Article  CAS  PubMed  Google Scholar 

  20. Xu, X. et al. Ferromagnetic-antiferromagnetic coexisting ground state and exchange bias effects in MnBi4Te7 and MnBi6Te10. Nat. Commun. 13, 7646 (2022).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  21. Phan, M.-H. et al. Exchange bias and interface-related effects in two-dimensional van der Waals magnetic heterostructures: open questions and perspectives. J. Alloy. Compd. 937, 168375 (2023).

    Article  CAS  Google Scholar 

  22. Song, T. et al. Direct visualization of magnetic domains and moiré magnetism in twisted 2D magnets. Science 374, 1140–1144 (2021).

    Article  CAS  PubMed  Google Scholar 

  23. Li, S. et al. Observation of stacking engineered magnetic phase transitions within moiré supercells of twisted van der Waals magnets. Nat. Commun. 15, 5712 (2024).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  24. Thiel, L. et al. Probing magnetism in 2D materials at the nanoscale with single-spin microscopy. Science 364, 973–976 (2019).

    Article  CAS  PubMed  Google Scholar 

  25. Tan, A. K. C. et al. Revealing emergent magnetic charge in an antiferromagnet with diamond quantum magnetometry. Nat. Mater. 23, 205–211 (2024).

    Article  CAS  PubMed  Google Scholar 

  26. Tschudin, M. A. et al. Imaging nanomagnetism and magnetic phase transitions in atomically thin CrSBr. Nat. Commun. 15, 6005 (2024).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  27. Palm, M. L. et al. Observation of current whirlpools in graphene at room temperature. Science 384, 465–469 (2024).

    Article  CAS  PubMed  Google Scholar 

  28. Sass, P. M., Kim, J., Vanderbilt, D., Yan, J. & Wu, W. Robust A-type order and spin–flop transition on the surface of the antiferromagnetic topological insulator MnBi2Te4. Phys. Rev. Lett. 125, 037201 (2020).

    Article  CAS  PubMed  Google Scholar 

  29. Sun, Z. et al. Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3. Nature 572, 497–501 (2019).

    Article  CAS  PubMed  Google Scholar 

  30. Zhong, D. et al. Layer-resolved magnetic proximity effect in van der Waals heterostructures. Nat. Nanotechnol. 15, 187–191 (2020).

    Article  CAS  PubMed  Google Scholar 

  31. Qiu, J.-X. et al. Axion optical induction of antiferromagnetic order. Nat. Mater. 22, 583–590 (2023).

    Article  CAS  PubMed  Google Scholar 

  32. Calder, S. et al. Magnetic structure and exchange interactions in the layered semiconductor CrPS4. Phys. Rev. B 102, 024408 (2020).

    Article  CAS  Google Scholar 

  33. Peng, Y. et al. Magnetic structure and metamagnetic transitions in the van der Waals antiferromagnet CrPS4. Adv. Mater. 32, 2001200 (2020).

    Article  CAS  Google Scholar 

  34. Son, J. et al. Air-stable and layer-dependent ferromagnetism in atomically thin van der Waals CrPS4. ACS Nano 15, 16904–16912 (2021).

    Article  CAS  PubMed  Google Scholar 

  35. Wu, F. et al. Gate-controlled magnetotransport and electrostatic modulation of magnetism in 2D magnetic semiconductor CrPS4. Adv. Mater. 35, 2211653 (2023).

    Article  CAS  Google Scholar 

  36. Lee, J. et al. Structural and optical properties of single- and few-layer magnetic semiconductor CrPS4. ACS Nano 11, 10935–10944 (2017).

    Article  CAS  PubMed  Google Scholar 

  37. Huang, M. et al. Layer-dependent magnetism and spin fluctuations in atomically thin van der Waals magnet CrPS4. Nano Lett. 23, 8099–8105 (2023).

    Article  CAS  PubMed  Google Scholar 

  38. Zur, Y. et al. Magnetic imaging and domain nucleation in CrSBr down to the 2D limit. Adv. Mater. 35, 2307195 (2023).

    Article  CAS  Google Scholar 

  39. Gao, A. et al. An antiferromagnetic diode effect in even-layered MnBi2Te4. Nat. Electron. 7, 751–759 (2024).

    Article  CAS  Google Scholar 

  40. Zhang, X.-Y. et al. Enhanced magnetization by defect-assisted exciton recombination in atomically thin CrCl3. Phys. Rev. Mater. 8, 104402 (2024).

    Article  CAS  Google Scholar 

  41. Guo, X. et al. Extraordinary phase transition revealed in a van der Waals antiferromagnet. Nat. Commun. 15, 6472 (2024).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  42. Jiang, S., Shan, J. & Mak, K. F. Electric-field switching of two-dimensional van der Waals magnets. Nat. Mater. 17, 406–410 (2018).

    Article  CAS  PubMed  Google Scholar 

  43. Hedrich, N. et al. Nanoscale mechanics of antiferromagnetic domain walls. Nat. Phys. 17, 574–577 (2021).

    Article  CAS  Google Scholar 

  44. Makushko, P. et al. Flexomagnetism and vertically graded Néel temperature of antiferromagnetic Cr2O3 thin films. Nat. Commun. 13, 6745 (2022).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  45. Wörnle, M. S. et al. Coexistence of Bloch and Néel walls in a collinear antiferromagnet. Phys. Rev. B 103, 094426 (2021).

    Article  Google Scholar 

  46. Hubert, A. and Schäfer, R. Magnetic Domains: The Analysis of Magnetic Microstructures, 141–142 (Springer, 1998).

  47. Shi, P. et al. Magnetoresistance oscillations in vertical junctions of 2D antiferromagnetic semiconductor CrPS4. Phys. Rev. X 14, 041065 (2024).

    CAS  Google Scholar 

  48. Wang, Z. et al. Determining the phase diagram of atomically thin layered antiferromagnet CrCl3. Nat. Nanotechnol. 14, 1116–1122 (2019).

    Article  PubMed  Google Scholar 

  49. Blundell, S. Magnetism in Condensed Matter, 134 (Oxford University Press, 2001).

  50. Beckmann, B., Nowak, U. & Usadel, K. D. Asymmetric reversal modes in ferromagnetic/antiferromagnetic multilayers. Phys. Rev. Lett. 91, 187201 (2003).

    Article  CAS  PubMed  Google Scholar 

  51. Ambrose, T., Sommer, R. L. & Chien, C. L. Angular dependence of exchange coupling in ferromagnet/antiferromagnet bilayers. Phys. Rev. B 56, 83–86 (1997).

    Article  CAS  Google Scholar 

  52. Xi, H., Kryder, M. H. & White, R. M. Study of the angular-dependent exchange coupling between a ferromagnetic and an antiferromagnetic layer. Appl. Phys. Lett. 74, 2687–2689 (1999).

    Article  CAS  Google Scholar 

  53. Liu, Z. et al. Strong lateral exchange coupling and current-induced switching in single-layer ferrimagnetic films with patterned compensation temperature. Phys. Rev. B 107, L100412 (2023).

    Article  CAS  Google Scholar 

  54. Hadjoudja, A., Garcia-Sanchez, F. & Lopez-Diaz, L. Interlayer coupled domain wall dynamics induced by external magnetic field in synthetic antiferromagnets. J. Phys. D: Appl. Phys. 57, 395006 (2024).

    Article  CAS  Google Scholar 

  55. Yang, S.-H., Ryu, K.-S. & Parkin, S. Domain-wall velocities of up to 750 m s−1 driven by exchange-coupling torque in synthetic antiferromagnets. Nat. Nanotechnol. 10, 221–226 (2015).

    Article  CAS  PubMed  Google Scholar 

  56. Sun, Z. et al. Resolving and routing magnetic polymorphs in a 2D layered antiferromagnet. Nat. Mater. 24, 226–233 (2025).

    Article  CAS  PubMed  Google Scholar 

  57. Pellet-Mary, C. et al. Lateral exchange bias for Néel-vector control in atomically thin antiferromagnets. Preprint at http://arxiv.org/abs/2503.04922 (2025).

  58. Bud’ko, S. L., Gati, E., Slade, T. J. & Canfield, P. C. Magnetic order in the van der Waals antiferromagnet CrPS4: anisotropic H–T phase diagrams and effects of pressure. Phys. Rev. B 103, 224407 (2021).

    Article  Google Scholar 

  59. Beg, M., Lang, M. & Fangohr, H. Ubermag: toward more effective micromagnetic workflows. IEEE Trans. Magn. 58, 7300205 (2022).

    Article  Google Scholar 

  60. Donahue, M. J. and Porter, D. G. OOMMF User’s Guide, Version 1.0, Technical Report (National Institute of Standards and Technology, 1999); https://doi.org/10.6028/NIST.IR.6376

  61. Evans, R. F. L. et al. Atomistic spin model simulations of magnetic nanomaterials. J. Phys. Condens. Matter 26, 103202 (2014).

    Article  CAS  PubMed  Google Scholar 

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Acknowledgements

The authors thank Y. Ran, P. Aynajian for valuable discussions and Q. Ma and K. S. Burch for use of some laboratory facilities. B.B.Z. and Y.-X.W. acknowledge support from the Department of Energy Early Career Program under award number DE-SC0024177 for NV centre measurements. B.B.Z., Y.-X.W. and T.K.M.G. acknowledge support from the National Science Foundation (NSF) award DMR-2047214 for development of the scanning NV microscope. B.B.Z. and X.-Y.Z. were supported by NSF ECCS-2041779 for sample fabrication and magnetization analysis. Z.L., M.A.I., R.N.G., G.P.T. and T.A. acknowledge a start-up fund from Binghamton University. Funding for the ADL Small Grants Program is made possible by support to S3IP from New York Empire State Development Division of Science, Technology, and Research. E.J.G.S. acknowledges computational resources through CIRRUS Tier-2 HPC Service (ec131 Cirrus Project) at EPCC, which is funded by the University of Edinburgh and EPSRC (EP/P020267/1); and ARCHER2 UK National Supercomputing Service via the UKCP consortium (Project e89) funded by EPSRC grant reference EP/X035891/1. E.J.G.S. acknowledges the EPSRC Open Fellowship (EP/T021578/1) and the Donostia International Physics Center for funding support. E.J.G.S. and R.R.-E. acknowledge support from the Royal Society through the International Newton Fellowship (NIF/R1/241532). K.W. and T.T. acknowledge support from the JSPS KAKENHI (grant numbers 21H05233 and 23H02052) and the World Premier International Research Center Initiative (WPI), MEXT, Japan.

Author information

Authors and Affiliations

  1. Department of Physics, Boston College, Chestnut Hill, MA, USA

    Yu-Xuan Wang, Thomas K. M. Graham, Xin-Yue Zhang & Brian B. Zhou

  2. Donostia International Physics Center (DIPC), Donostia-San Sebastián, Spain

    Ricardo Rama-Eiroa & Elton J. G. Santos

  3. Institute for Condensed Matter and Complex Systems, School of Physics and Astronomy, University of Edinburgh, Edinburgh, UK

    Ricardo Rama-Eiroa, Mohammad H. Badarneh & Elton J. G. Santos

  4. Department of Physics, Applied Physics and Astronomy, Binghamton University, Binghamton, NY, USA

    Md Ariful Islam, Rafael Nunes Gontijo, Ganesh Prasad Tiwari, Tibendra Adhikari & Zhong Lin

  5. Research Center for Electronic and Optical Materials, National Institute for Materials Science, Tsukuba, Japan

    Kenji Watanabe

  6. Research Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan

    Takashi Taniguchi

  7. Department of Chemistry, Binghamton University, Binghamton, NY, USA

    Claire Besson

  8. Higgs Centre for Theoretical Physics, University of Edinburgh, Edinburgh, UK

    Elton J. G. Santos

  9. Materials Science and Engineering Program, Binghamton University, Binghamton, NY, USA

    Zhong Lin

Authors
  1. Yu-Xuan Wang
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Contributions

Y.-X.W., Z.L. and B.B.Z. conceived the experiments. M.A.I. and G.P.T. synthesized the bulk crystals. M.A.I., R.N.G., G.P.T. and T.A. performed bulk crystal characterizations and RMCD measurements. C.B. performed X-ray diffraction measurements. Z.L. supervised the research at Binghamton University. Y.-X.W. and T.K.M.G. developed the scanning NV magnetometry instrumentation and protocols. Y.-X.W. fabricated the samples and performed the scanning NV experiments, with the assistance of T.K.M.G. and X.-Y.Z. Y.-X.W. analysed the data and performed micromagnetic simulations, with the assistance of X.-Y.Z. and B.B.Z. Atomistic spin dynamics simulations were performed by R.R.-E., and the Stoner–Wohlfarth model was developed by M.H.B., both under the guidance of E.J.G.S. K.W. and T.T. synthesized the hexagonal boron nitride crystals. B.B.Z., Y.-X.W., R.R.-E., M.H.B. and E.J.G.S. wrote the manuscript, with input from all authors.

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Correspondence to Brian B. Zhou.

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Supplementary information

Supplementary Information (download PDF )

Supplementary Figs. 1–21, Tables 1–3 and Discussion.

Supplementary Video 1 (download MP4 )

Video of the dynamical evolution of a thermally nucleated even-layer domain wall in atomistic simulations at an applied magnetic field of +200 mT. The video plots the components of the total magnetization summed over all layers.

Supplementary Video 2 (download MP4 )

Same simulation as Supplementary Video 1 at +200 mT, but the magnetization components of only the third layer are plotted.

Supplementary Video 3 (download MP4 )

Video of the dynamical evolution of a thermally nucleated even-layer domain wall in atomistic simulations at an applied magnetic field of − 200 mT. The video plots the components of the total magnetization summed over all layers.

Supplementary Video 4 (download MP4 )

Same simulation as Supplementary Video 3 at − 200 mT, but the magnetization components of only the third layer are plotted.

Source data

Source Data Fig. 1 (download XLSX )

Statistical source data and analysed reconstruction data.

Source Data Fig. 2 (download XLSX )

Statistical source data.

Source Data Fig. 3 (download XLSX )

Statistical source data and classified hysteresis data.

Source Data Fig. 4 (download XLSX )

Statistical source data and classified hysteresis data.

Source Data Fig. 5 (download XLSX )

Statistical source data and classified hysteresis data.

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Wang, YX., Graham, T.K.M., Rama-Eiroa, R. et al. Configurable antiferromagnetic domains and lateral exchange bias in atomically thin CrPS4. Nat. Mater. 24, 1414–1423 (2025). https://doi.org/10.1038/s41563-025-02259-x

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