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Interferroic magnetoelectric coupling at CuCrP2S6/Fe3GeTe2 van der Waals heterojunctions

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.

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Fig. 1: 2D vdW FE/FM multiferroic heterostructure device.
Fig. 2: Ferroelectricity in CCPS and ITO/CCPS/FGT FTJ.
Fig. 3: FE control of magnetism in a CCPS/FGT multiferroic heterostructure device.
Fig. 4: FE control of 2D FGT of varying thicknesses and DFT calculations of CCPS/FGT heterostructures.

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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.

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The codes used for plotting the data are available from the corresponding author upon reasonable request.

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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.

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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 PE 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.

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Correspondence to Cheng Gong.

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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

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