Tailorable multiferroic tunnel junctions from all-van der Waals multilayer stacking

Ti Xie; Qinqin Wang; Hongrui Zhang; Khimananda Acharya; Ju Chen; Chen Liu; Zhihao Song; Samuel August Deitemyer; Hasitha Suriya Arachchige; Qishuo Tan; Andrew F. May; Seng Huat Lee; Michael A. Susner; Zhiqiang Mao; Michael A. McGuire; Xi Ling; David Mandrus; Xixiang Zhang; Shi Jing Gong; Tula R. Paudel; Ramamoorthy Ramesh; Evgeny Y. Tsymbal; Cheng Gong

doi:10.1038/s41565-025-02065-1

Tailorable multiferroic tunnel junctions from all-van der Waals multilayer stacking

Ti Xie
, Qinqin Wang
, Hongrui Zhang
, Khimananda Acharya
, Ju Chen
, Chen Liu
, Zhihao Song
, Samuel August Deitemyer
, Hasitha Suriya Arachchige
, Qishuo Tan
, Andrew F. May
, Seng Huat Lee
, Michael A. Susner
, Zhiqiang Mao
, Michael A. McGuire
, Xi Ling
, David Mandrus
, Xixiang Zhang
, Shi Jing Gong
, Tula R. Paudel

Ramamoorthy Ramesh, Evgeny Y. Tsymbal, Cheng Gong

Correlated Electron Materials

Research output: Contribution to journal › Article › peer-review

12 Scopus citations

Abstract

Multiferroic tunnel junctions (MFTJs) represent a class of multistate, non-volatile spintronic devices, in which electron tunnelling can be manipulated by switching long-range lattice and spin orders. In contrast to conventional oxide-based MFTJs, MFTJs constructed from two-dimensional van der Waals (vdW) crystals promise minimal defect concentration in the constituents and at interfaces, which may allow for probing intrinsic tunnelling physics and the development of high-performance devices. Here we construct Fe₃GeTe₂/CuInP₂S₆/Fe₃GeTe₂ all-vdW MFTJs by assembling multilayer flakes of ferromagnetic Fe₃GeTe₂ electrodes and a ferroelectric CuInP₂S₆ spacer. These MFTJs exhibit four non-volatile resistance states featuring sizable tunnelling magnetoresistance of ∼10²% and tunnelling electroresistance of ∼10⁴%. To tune the properties of the vdW MFTJ, we make use of the flexibility in material choice offered by vdW heterostructure devices; we use Fe₃GeTe₂/Fe₅GeTe₂ asymmetric electrodes to boost the tunnelling electroresistance by 10³%, we integrate In₂Se₃ as a ferroelectric with a smaller bandgap to enhance the ON-state current density by 10⁴% to 10⁴ A cm⁻² and we use Fe₃GaTe₂ electrodes to demonstrate room temperature operation. Furthermore, when we combine the asymmetric ferromagnetic electrodes with the small-bandgap ferroelectric spacer to construct Fe₃GeTe₂/In₂Se₃/Fe₅GeTe₂ MFTJs, we simultaneously realized tunnelling electroresistance of 10⁶% and an ON-state current density of 10⁴ A cm⁻², both two orders of magnitude higher than the highest values achieved with conventional oxide-based MFTJs. In the future, our all-vdW MFTJs with the tailorability of all functional layers may make it possible to investigate fundamental aspects of interlayer tunnelling and enable the design of functional magnetoelectric nanodevices.

Original language	English
Pages (from-to)	366-373
Number of pages	8
Journal	Nature Nanotechnology
Volume	21
Issue number	3
DOIs	https://doi.org/10.1038/s41565-025-02065-1
State	Published - Mar 2026

Funding

C.G. acknowledges the support from Air Force Office of Scientific Research (grant number 326 FA9550-22-1-0349) and Office of Naval Research (grant number N000142612040). MFTJ device fabrication was supported by the Naval Air Warfare Center Aircraft Division (grant number N00421-22-1-0001) and the Army Research Laboratory (cooperative agreement number W911NF-19-2-0181). Electrical transport measurements, RMCD measurements, Raman spectroscopic measurements and AFM measurements were supported by the National Science Foundation (grant numbers DMR-2326944, DMR-2340773, FuSe-2425599 and ECCS-2429994). E.Y.T. acknowledges grant support from the US Department of Energy, Office of Science, Basic Energy Sciences (grant number DE-SC0023140). Crystal synthesis and characterization by A.F.M., H.S.A., D.M. and M.A.M. was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. T.R.P. acknowledges grant support from the National Science Foundation, Established Program to Stimulate Competitive Research, Research Infrastructure Improvement Track-1: Emergent Quantum Materials and Technologies Award, OIA-2329159. M.A.S. acknowledges support through the United States Air Force Office of Scientific Research LRIR23RXCOR003 and AOARD—MOST (grant number F4GGA21207H002). S.H.L. and Z.M. acknowledge support from the National Science Foundation through the Penn State 2D Crystal Consortium—Materials Innovation Platform (2DCC-MIP) (cooperative agreement number DMR-2039351).

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Xie, T., Wang, Q., Zhang, H., Acharya, K., Chen, J., Liu, C., Song, Z., Deitemyer, S. A., Arachchige, H. S., Tan, Q., May, A. F., Lee, S. H., Susner, M. A., Mao, Z., McGuire, M. A., Ling, X., Mandrus, D., Zhang, X., Gong, S. J., ... Gong, C. (2026). Tailorable multiferroic tunnel junctions from all-van der Waals multilayer stacking. Nature Nanotechnology, 21(3), 366-373. https://doi.org/10.1038/s41565-025-02065-1

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title = "Tailorable multiferroic tunnel junctions from all-van der Waals multilayer stacking",

abstract = "Multiferroic tunnel junctions (MFTJs) represent a class of multistate, non-volatile spintronic devices, in which electron tunnelling can be manipulated by switching long-range lattice and spin orders. In contrast to conventional oxide-based MFTJs, MFTJs constructed from two-dimensional van der Waals (vdW) crystals promise minimal defect concentration in the constituents and at interfaces, which may allow for probing intrinsic tunnelling physics and the development of high-performance devices. Here we construct Fe3GeTe2/CuInP2S6/Fe3GeTe2 all-vdW MFTJs by assembling multilayer flakes of ferromagnetic Fe3GeTe2 electrodes and a ferroelectric CuInP2S6 spacer. These MFTJs exhibit four non-volatile resistance states featuring sizable tunnelling magnetoresistance of ∼102\% and tunnelling electroresistance of ∼104\%. To tune the properties of the vdW MFTJ, we make use of the flexibility in material choice offered by vdW heterostructure devices; we use Fe3GeTe2/Fe5GeTe2 asymmetric electrodes to boost the tunnelling electroresistance by 103\%, we integrate In2Se3 as a ferroelectric with a smaller bandgap to enhance the ON-state current density by 104\% to 104 A cm−2 and we use Fe3GaTe2 electrodes to demonstrate room temperature operation. Furthermore, when we combine the asymmetric ferromagnetic electrodes with the small-bandgap ferroelectric spacer to construct Fe3GeTe2/In2Se3/Fe5GeTe2 MFTJs, we simultaneously realized tunnelling electroresistance of 106\% and an ON-state current density of 104 A cm−2, both two orders of magnitude higher than the highest values achieved with conventional oxide-based MFTJs. In the future, our all-vdW MFTJs with the tailorability of all functional layers may make it possible to investigate fundamental aspects of interlayer tunnelling and enable the design of functional magnetoelectric nanodevices.",

author = "Ti Xie and Qinqin Wang and Hongrui Zhang and Khimananda Acharya and Ju Chen and Chen Liu and Zhihao Song and Deitemyer, \{Samuel August\} and Arachchige, \{Hasitha Suriya\} and Qishuo Tan and May, \{Andrew F.\} and Lee, \{Seng Huat\} and Susner, \{Michael A.\} and Zhiqiang Mao and McGuire, \{Michael A.\} and Xi Ling and David Mandrus and Xixiang Zhang and Gong, \{Shi Jing\} and Paudel, \{Tula R.\} and Ramamoorthy Ramesh and Tsymbal, \{Evgeny Y.\} and Cheng Gong",

note = "Publisher Copyright: {\textcopyright} The Author(s), under exclusive licence to Springer Nature Limited 2026.",

year = "2026",

month = mar,

doi = "10.1038/s41565-025-02065-1",

language = "English",

volume = "21",

pages = "366--373",

journal = "Nature Nanotechnology",

issn = "1748-3387",

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Xie, T, Wang, Q, Zhang, H, Acharya, K, Chen, J, Liu, C, Song, Z, Deitemyer, SA, Arachchige, HS, Tan, Q, May, AF, Lee, SH, Susner, MA, Mao, Z, McGuire, MA, Ling, X, Mandrus, D, Zhang, X, Gong, SJ, Paudel, TR, Ramesh, R, Tsymbal, EY & Gong, C 2026, 'Tailorable multiferroic tunnel junctions from all-van der Waals multilayer stacking', Nature Nanotechnology, vol. 21, no. 3, pp. 366-373. https://doi.org/10.1038/s41565-025-02065-1

TY - JOUR

T1 - Tailorable multiferroic tunnel junctions from all-van der Waals multilayer stacking

AU - Xie, Ti

AU - Wang, Qinqin

AU - Zhang, Hongrui

AU - Acharya, Khimananda

AU - Chen, Ju

AU - Liu, Chen

AU - Song, Zhihao

AU - Deitemyer, Samuel August

AU - Arachchige, Hasitha Suriya

AU - Tan, Qishuo

AU - May, Andrew F.

AU - Lee, Seng Huat

AU - Susner, Michael A.

AU - Mao, Zhiqiang

AU - McGuire, Michael A.

AU - Ling, Xi

AU - Mandrus, David

AU - Zhang, Xixiang

AU - Gong, Shi Jing

AU - Paudel, Tula R.

AU - Ramesh, Ramamoorthy

AU - Tsymbal, Evgeny Y.

AU - Gong, Cheng

PY - 2026/3

Y1 - 2026/3

N2 - Multiferroic tunnel junctions (MFTJs) represent a class of multistate, non-volatile spintronic devices, in which electron tunnelling can be manipulated by switching long-range lattice and spin orders. In contrast to conventional oxide-based MFTJs, MFTJs constructed from two-dimensional van der Waals (vdW) crystals promise minimal defect concentration in the constituents and at interfaces, which may allow for probing intrinsic tunnelling physics and the development of high-performance devices. Here we construct Fe3GeTe2/CuInP2S6/Fe3GeTe2 all-vdW MFTJs by assembling multilayer flakes of ferromagnetic Fe3GeTe2 electrodes and a ferroelectric CuInP2S6 spacer. These MFTJs exhibit four non-volatile resistance states featuring sizable tunnelling magnetoresistance of ∼102% and tunnelling electroresistance of ∼104%. To tune the properties of the vdW MFTJ, we make use of the flexibility in material choice offered by vdW heterostructure devices; we use Fe3GeTe2/Fe5GeTe2 asymmetric electrodes to boost the tunnelling electroresistance by 103%, we integrate In2Se3 as a ferroelectric with a smaller bandgap to enhance the ON-state current density by 104% to 104 A cm−2 and we use Fe3GaTe2 electrodes to demonstrate room temperature operation. Furthermore, when we combine the asymmetric ferromagnetic electrodes with the small-bandgap ferroelectric spacer to construct Fe3GeTe2/In2Se3/Fe5GeTe2 MFTJs, we simultaneously realized tunnelling electroresistance of 106% and an ON-state current density of 104 A cm−2, both two orders of magnitude higher than the highest values achieved with conventional oxide-based MFTJs. In the future, our all-vdW MFTJs with the tailorability of all functional layers may make it possible to investigate fundamental aspects of interlayer tunnelling and enable the design of functional magnetoelectric nanodevices.

AB - Multiferroic tunnel junctions (MFTJs) represent a class of multistate, non-volatile spintronic devices, in which electron tunnelling can be manipulated by switching long-range lattice and spin orders. In contrast to conventional oxide-based MFTJs, MFTJs constructed from two-dimensional van der Waals (vdW) crystals promise minimal defect concentration in the constituents and at interfaces, which may allow for probing intrinsic tunnelling physics and the development of high-performance devices. Here we construct Fe3GeTe2/CuInP2S6/Fe3GeTe2 all-vdW MFTJs by assembling multilayer flakes of ferromagnetic Fe3GeTe2 electrodes and a ferroelectric CuInP2S6 spacer. These MFTJs exhibit four non-volatile resistance states featuring sizable tunnelling magnetoresistance of ∼102% and tunnelling electroresistance of ∼104%. To tune the properties of the vdW MFTJ, we make use of the flexibility in material choice offered by vdW heterostructure devices; we use Fe3GeTe2/Fe5GeTe2 asymmetric electrodes to boost the tunnelling electroresistance by 103%, we integrate In2Se3 as a ferroelectric with a smaller bandgap to enhance the ON-state current density by 104% to 104 A cm−2 and we use Fe3GaTe2 electrodes to demonstrate room temperature operation. Furthermore, when we combine the asymmetric ferromagnetic electrodes with the small-bandgap ferroelectric spacer to construct Fe3GeTe2/In2Se3/Fe5GeTe2 MFTJs, we simultaneously realized tunnelling electroresistance of 106% and an ON-state current density of 104 A cm−2, both two orders of magnitude higher than the highest values achieved with conventional oxide-based MFTJs. In the future, our all-vdW MFTJs with the tailorability of all functional layers may make it possible to investigate fundamental aspects of interlayer tunnelling and enable the design of functional magnetoelectric nanodevices.

UR - https://www.scopus.com/pages/publications/105031131106

U2 - 10.1038/s41565-025-02065-1

DO - 10.1038/s41565-025-02065-1

M3 - Article

AN - SCOPUS:105031131106

SN - 1748-3387

VL - 21

SP - 366

EP - 373

JO - Nature Nanotechnology

JF - Nature Nanotechnology

IS - 3

ER -

Tailorable multiferroic tunnel junctions from all-van der Waals multilayer stacking

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