Abstract
Two-dimensional materials that combine ferroelectric and ferromagnetic orders could exhibit a range of exotic physical properties and find use in applications such as energy-efficient spintronics. However, long-range ferroic orders in two dimensions are prone to destruction. For example, depolarization fields can destabilize ferroelectric order and thermal fluctuations can suppress magnetic order. Here we report multiferroic van der Waals heterostructures made from atomic layers of ferroelectric CuCrP2S6 and ferromagnetic Fe3GeTe2. We demonstrate reversible, non-volatile ferroelectric control of the magnetic anisotropy of two-dimensional Fe3GeTe2, and with this, probe the interferroic magnetoelectric coupling. Polarization switching of CuCrP2S6 changes the magnetic coercivity of a 3.8-nm-thick Fe3GeTe2 layer by approximately 14 mT at a testing temperature of 153 K, with a control efficiency around 65%. The control efficiency decreases as the Fe3GeTe2 thickness increases due to the short-range interfacial magnetoelectric coupling of the heterostructure multiferroicity.
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
$32.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 digital issues and online access to articles
$119.00 per year
only $9.92 per issue
Buy this article
- Purchase on SpringerLink
- Instant access to the full article PDF.
USD 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. Other data that support the findings of this study are available from the corresponding author upon reasonable request.
Code availability
The codes used for plotting the data are available from the corresponding author upon reasonable request.
References
Spaldin, N. A. & Ramesh, R. Advances in magnetoelectric multiferroics. Nat. Mater. 18, 203–212 (2019).
Mundy, J. A. et al. Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic. Nature 537, 523–527 (2016).
Song, Q. et al. Evidence for a single-layer van der Waals multiferroic. Nature 602, 601–605 (2022).
Seixas, L., Rodin, A. S., Carvalho, A. & Castro Neto, A. H. Multiferroic two-dimensional materials. Phys. Rev. Lett. 116, 206803 (2016).
Chu, Y.-H. et al. Electric-field control of local ferromagnetism using a magnetoelectric multiferroic. Nat. Mater. 7, 478–482 (2008).
Baek, S. H. et al. Ferroelastic switching for nanoscale non-volatile magnetoelectric devices. Nat. Mater. 9, 309–314 (2010).
Manipatruni, S. et al. Scalable energy-efficient magnetoelectric spin-orbit logic. Nature 565, 35–42 (2019).
Stamm, C. et al. Magneto-optical detection of the spin Hall effect in Pt and W thin films. Phys. Rev. Lett. 119, 087203 (2017).
Linder, J. & Robinson, J. W. A. Superconducting spintronics. Nat. Phys. 11, 307–315 (2015).
Ahn, E. C. 2D materials for spintronic devices. npj 2D Mater. Appl. 4, 17 (2020).
Mak, K. F., Xiao, D. & Shan, J. Light-valley interactions in 2D semiconductors. Nat. Photon. 12, 451–460 (2018).
Wang, Y. et al. Electric-field-driven non-volatile multi-state switching of individual skyrmions in a multiferroic heterostructure. Nat. Commun. 11, 3577 (2020).
Fiebig, M., Lottermoser, T., Meier, D. & Trassin, M. The evolution of multiferroics. Nat. Rev. Mater. 1, 16046 (2016).
Du, R. et al. Two-dimensional multiferroic material of metallic p-doped SnSe. Nat. Commun. 13, 6130 (2022).
Pacchioni, G. et al. A design strategy for 2D multiferroics. Nat. Rev. Mater. 8, 9 (2023).
Wu, D. et al. Thickness-dependent dielectric constant of few-layer In2Se3 nanoflakes. Nano Lett. 15, 8136–8140 (2015).
Liu, F. et al. Room-temperature ferroelectricity in CuInP2S6 ultrathin flakes. Nat. Commun. 7, 12357 (2016).
Fei, R., Kang, W. & Yang, L. Ferroelectricity and phase transitions in monolayer group-IV monochalcogenides. Phys. Rev. Lett. 117, 097601 (2016).
Gong, C. et al. Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals. Nature 546, 265–269 (2017).
Huang, B. et al. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. Nature 546, 270–273 (2017).
Gong, C. & Zhang, X. Two-dimensional magnetic crystals and emergent heterostructure devices. Science 363, eaav4450 (2019).
Novoselov, K. S., Mishchenko, A., Carvalho, A. & Castro Neto, A. H. 2D materials and van der Waals heterostructures. Science 353, aac9439 (2016).
Geim, A. K. & Grigorieva, I. V. Van der Waals heterostructures. Nature 499, 419–425 (2013).
Duan, C.-G. et al. Surface magnetoelectric effect in ferromagnetic metal films. Phys. Rev. Lett. 101, 137201 (2008).
Gong, C., Kim, E. M., Wang, Y., Lee, G. & Zhang, X. Multiferroicity in atomic van der Waals heterostructures. Nat. Commun. 10, 2657 (2019).
Huang, C. et al. Toward room-temperature electrical control of magnetic order in multiferroic van der Waals materials. Nano Lett. 22, 5191–5197 (2022).
Heron, J. T. et al. Electric-field-induced magnetization reversal in a ferromagnet-multiferroic heterostructure. Phys. Rev. Lett. 107, 217202 (2011).
Weisheit, M. et al. Electric field-induced modification of magnetism in thin-film ferromagnets. Science 315, 349–351 (2007).
Dankert, A. & Dash, S. P. Electrical gate control of spin current in van der Waals heterostructures at room temperature. Nat. Commun. 8, 16093 (2017).
Sun, W. et al. Controlling bimerons as skyrmion analogues by ferroelectric polarization in 2D van der Waals multiferroic heterostructures. Nat. Commun. 11, 5930 (2020).
Wang, X. et al. Electrical and magnetic anisotropies in van der Waals multiferroic CuCrP2S6. Nat. Commun. 14, 840 (2023).
Deng, Y. et al. Gate-tunable room-temperature ferromagnetism in two-dimensional Fe3GeTe2. Nature 563, 94–99 (2018).
Wu, J. et al. High tunneling electroresistance in a ferroelectric van der Waals heterojunction via giant barrier height modulation. Nat. Electron. 3, 466–472 (2020).
Wang, Q. et al. Extraordinary tunnel electroresistance in layer-by-layer engineered van der Waals ferroelectric tunnel junctions. Matter 5, 4425–4436 (2022).
Wu, M. & Li, J. Sliding ferroelectricity in 2D van der Waals materials: related physics and future opportunities. Proc. Natl Acad. Sci. USA 118, e2115703118 (2021).
Rao, R., Conner, B. S., Jiang, J., Pachter, R. & Susner, M. A. Raman spectroscopy study of pressure-induced phase transitions in single crystal CuInP2S6. J. Chem. Phys. 159, 224706 (2023).
Susner, M. A., Rao, R., Pelton, A. T., McLeod, M. V. & Maruyama, B. Temperature-dependent Raman scattering and X-ray diffraction study of phase transitions in layered multiferroic CuCrP2S6. Phys. Rev. Mater. 4, 104003 (2020).
Liang, S. et al. Small-voltage multiferroic control of two-dimensional magnetic insulators. Nat. Electron. 6, 199–205 (2023).
Park, C. B. et al. Observation of spin‐induced ferroelectricity in a layered van der Waals antiferromagnet CuCrP2S6. Adv. Electron. Mater. 8, 2101072 (2022).
Lai, Y. et al. Two-dimensional ferromagnetism and driven ferroelectricity in van der Waals CuCrP2S6. Nanoscale 11, 5163–5170 (2019).
Ma, Y. et al. High-performance van der Waals antiferroelectric CuCrP2S6-based memristors. Nat. Commun. 14, 7891 (2023).
Hu, J.-M., Chen, L.-Q. & Nan, C.-W. Multiferroic heterostructures integrating ferroelectric and magnetic materials. Adv. Mater. 28, 15–39 (2016).
Coey, J. M. D. Industrial applications of permanent magnetism. Phys. Scr. T66, 60–69 (1996).
Brehm, J. A. et al. Tunable quadruple-well ferroelectric van der Waals crystals. Nat. Mater. 19, 43–48 (2020).
Wang, K. et al. Interface-tuning of ferroelectricity and quadruple-well state in CuInP2S6 via ferroelectric oxide. ACS Nano 17, 15787–15795 (2023).
Ederer, C. & Spaldin, N. A. Weak ferromagnetism and magnetoelectric coupling in bismuth ferrite. Phys. Rev. B 71, 060401 (2005).
Duan, C.-G., Jaswal, S. S. & Tsymbal, E. Y. Predicted magnetoelectric effect in Fe/BaTiO3 multilayers: ferroelectric control of magnetism. Phys. Rev. Lett. 97, 047201 (2006).
Ravindran, P., Vidya, R., Kjekshus, A., Fjellvag, H. & Eriksson, O. Theoretical investigation of magnetoelectric behavior in BiFeO3. Phys. Rev. B 74, 224412 (2006).
Kim, D., Lee, C., Jang, B. G., Kim, K. & Shim, J. H. Drastic change of magnetic anisotropy in Fe3GeTe2 and Fe4GeTe2 monolayers under electric field studied by density functional theory. Sci. Rep. 11, 17567 (2021).
Yi, J. et al. Competing antiferromagnetism in a quasi-2D itinerant ferromagnet: Fe3GeTe2. 2D Mater. 4, 011005 (2016).
Castellanos-Gomez, A. et al. Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping. 2D Mater. 1, 011002 (2012).
Mohapatra, S., Weber, W., Bowen, M., Boukari, S. & Da Costa, V. Toward accurate ferroelectric polarization estimation in nanoscopic systems. J. Appl. Phys. 132, 134101 (2022).
Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953–17979 (1994).
Deiseroth, H.-J., Aleksandrov, K., Reiner, C., Kienle, L. & Kremer, R. K. Fe3GeTe2 and Ni3GeTe2—two new layered transition-metal compounds: crystal structures, HRTEM investigations, and magnetic and electrical properties. Eur. J. Inorg. Chem. 2006, 1561–1567 (2006).
Duan, X., Wang, H., Chen, X. & Qi, J. Multiple polarization phases and strong magnetoelectric coupling in the layered transition metal phosphorus chalcogenides TMP2X6 (T = Cu, Ag; M = Cr, V; X = S, Se) by controlling the interlayer interaction and dimension. Phys. Rev. B 106, 115403 (2022).
Perdew, J. P., McMullen, E. R. & Zunger, A. Density-functional theory of the correlation energy in atoms and ions: a simple analytic model and a challenge. Phys. Rev. A 23, 2785–2789 (1981).
Moellmann, J. & Grimme, S. DFT-D3 study of some molecular crystals. J. Phys. Chem. C 118, 7615–7621 (2014).
Acknowledgements
C.G. acknowledges grant support from the Air Force Office of Scientific Research (grant number FA9550-22-1-0349) and the Office of Naval Research (grant number N000142612040). Device fabrication carried out by S.L. was supported by the Naval Air Warfare Center Aircraft Division (grant number N00421-22-1-0001) and Army Research Laboratory (cooperative agreement number W911NF-19-2-0181) under the supervision of C.G. Electrical transport measurements, Raman spectroscopic measurements and RMCD measurements carried out by S.L. were supported by National Science Foundation (grant numbers CMMI-2233592, DMR-2340773, DMR-2326944, FuSe-2425599 and ECCS-2429994). S.L. also acknowledges support from the Hulka Energy Research Fellowship at the A. James Clark School of Engineering, University of Maryland, College Park. H.Z. and R.R. acknowledge the Air Force Office of Scientific Research 2D Materials and Devices Research program through Clarkson Aerospace Corp (grant number FA9550-21-1-0460). PFM measurements carried out by Y.M. were supported by King Abdullah University of Science and Technology (grant numbers ORA-CRG10-2021-4665 and ORA-CRG11-2022-5031) under the supervision of X.Z. PFM measurements conducted by O.P. and S.M.N. were supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility. DFT calculations conducted by B.X. were supported by a special fund for Science and Technology Innovation Teams of Shanxi Province (grant number 202204051001002) under the supervision of W.-H.W. B.X. and W.-H.W. acknowledge support from the Supercomputing Center of Nankai University for the computational resources and technical support. Crystal growth by M.A.S. and B.S.C. was supported by the Air Force Office of Scientific Research (grant number LRIR 23RXCOR003) and AOARD-MOST (grant number F4GGA21207H002). M.A.S. and B.S.C. also acknowledge general support from the Air Force Materials and Manufacturing (RX), Sensors (RY) and Aerospace Systems (RQ) Directorates.
Author information
Authors and Affiliations
Contributions
C.G. conceived and supervised the project. S.L. conducted the 2D sample exfoliation and device fabrication. S.L. performed the RMCD and electrical measurements under the supervision of C.G. Y.M. conducted the XRD, SHG and P–E measurements under the supervision of X.Z. Y.M., O.P. and S.M.N. conducted the PFM measurements. S.M.N., P.M., H.Z. and R.R. provided detailed data analysis of the PFM results. S.S. conducted the structural characterizations, including energy-dispersive X-ray spectroscopy, SAED and STEM, under the supervision of J.J.C. C.F. performed the low-temperature SHG measurements under the supervision of J.X. M.L.C. and T.E.M. contributed to the SHG measurements. B.X. conducted the DFT calculations under the supervision of W.-H.W. Y.W. conducted the DFT calculations under the supervision of C.G. and contributed to the discussion of the computational results. H.S.A. and D.M. synthesized the bulk single crystals of FGT. M.A.S. and B.S.C. synthesized the bulk single crystals of CCPS. S.L. and C.G. analysed the data and wrote the paper. All authors commented on the paper.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Electronics thanks Xueyun Wang, Li Yang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information (download PDF )
Supplementary Figs. 1–13, Tables 1 and 2 and Notes.
Source data
Source Data Fig. 1 (download XLSX )
Source data for Fig. 1.
Source Data Fig. 2 (download XLSX )
Source data for Fig. 2.
Source Data Fig. 3 (download XLSX )
Source data for Fig. 3.
Source Data Fig. 4 (download XLSX )
Source data for Fig. 4.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Liang, S., Ma, Y., Xin, B. et al. Interferroic magnetoelectric coupling at CuCrP2S6/Fe3GeTe2 van der Waals heterojunctions. Nat Electron 9, 23–32 (2026). https://doi.org/10.1038/s41928-025-01461-8
Received:
Accepted:
Published:
Version of record:
Issue date:
DOI: https://doi.org/10.1038/s41928-025-01461-8
This article is cited by
-
Van der Waals heterostructures go multiferroic
Nature Electronics (2026)


