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.
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Data availability
The authors declare that the data supporting the findings of this study are available within the paper. Additional information is available from the corresponding authors upon reasonable request. Source data are provided with this paper.
Code availability
The data analysis computer codes used in this study are available from the corresponding authors upon reasonable request.
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Acknowledgements
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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Contributions
C.G. conceived the project and designed experiments. Q.W. and T.X. fabricated the devices and performed the experiments, assisted by Z.S. and S.A.D. H.Z. performed PFM measurements and analysis under the supervision of R.R. K.A., T.R.P. and E.Y.T. calculated layer-dependent work functions of F3GT and F5GT and density of states for the multiferroic heterostructures. J.C. also calculated density of states for F3GT/CIPS and F3GT/In2Se3 under the supervision of S.-J.G. and C.G. C.L. performed cross-sectional scanning transmission electron microscopy and electron energy loss spectroscopy under the supervision of X.Z. H.S.A. synthesized F3GT crystals under the supervision of D.M. Q.T. synthesized CIPS crystals under the supervision of X.L. A.F.M. and M.A.M. synthesized and characterized F5GT crystals. S.H.L. synthesized In2Se3 crystals under the supervision of Z.M. M.A.S. synthesized FGaT crystals. T.X., Q.W., R.R., E.Y.T. and C.G. analysed the data. T.X., E.Y.T., R.R. and C.G. wrote the paper assisted by Q.W. and Z.S. All authors commented on the paper.
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Extended data
Extended Data Fig. 1 AFM characterizations of an F3GT/CIPS/F3GT heterostructure.
AFM height profiles measured along the red, yellow, and blue dashed lines in the left panel show the thicknesses of the top F3GT (~12.6 nm), middle CIPS (~5.1 nm), and bottom F3GT (~3.6 nm), respectively. To avoid the thickness-induced variance, the thicknesses of each component of all tested all-vdW MFTJs were selected to be similar to those of this MFTJ.
Extended Data Fig. 2 Cross-sectional scanning transmission electron microscopy images of the F3GT/CIPS interface.
The zoomed-in image reveals atomically sharp and clean interfaces between F3GT and CIPS, with no observable oxidation or contamination, which confirms that the dry transfer process is effective in preserving high-quality interfaces.
Extended Data Fig. 3 Electron energy loss spectroscopy images of F3GT/CIPS interface.
a, A cross-sectional scanning transmission electron microscopy image of the F3GT/CIPS interface. b–d, Electron energy loss spectroscopy intensity maps showing the elemental distributions of Fe and Cu (b), In (c), and P (d) edges. The results show no significant structural distortion or atomic interdiffusion across the interface. White dashed lines serve as visual guides.
Extended Data Fig. 4 Raman spectra of a CIPS flake and an F3GT flake.
For the Raman spectrum of CIPS in the left panel, the vibration of anion corresponds to the peak at ~100 cm−1, and the S-P-P bending mode corresponds to the peak at 160 cm−1. S-P-S bending and cation vibration are responsible for the peaks located at 262 and 316 cm−1, respectively. The vibrations of P-P and P-S correspond to the peaks at ~373 cm−1 and 450 cm−1, respectively. As for F3GT, the peaks at ~122 cm−1 and 155 cm−1 correspond to the A1g and A1g+E2g modes, respectively. These well-defined Raman peaks agree with the previous works on high-quality CIPS and F3GT crystals34,49, indicating the high crystalline quality of our flakes, which is critical for achieving high-performance MFTJs.
Extended Data Fig. 5 PFM measurements for CIPS/F3GT heterostructures.
a, Schematic illustration of the PFM measurements for the CIPS/F3GT heterostructure (Fig. 1d of the main text). The conductive substrate is a 50-nm-thick Au film deposited on a SiO2/Si chip, serving as a bottom electrode for PFM measurements. Voltages are applied between the top PFM tip and the bottom electrode to change the PFM amplitude and phase of the CIPS. b, Box-in-box writing in another CIPS/F3GT heterostructure by PFM. We assembled another CIPS/F3GT heterostructure featuring a large overlap area for box-in-box writing. Left: Optical image of a 148-nm-thick CIPS flake (circled by white dashed lines) on a bulk F3GT (circled by black dashed lines) flake. Green boxes indicate the regions for applying writing voltages. Right: PFM phase image of a CIPS/F3GT heterostructure with a written box-in-box pattern. A −10 V d.c. bias voltage was applied in the inner green box, and a +10 V d.c. bias voltage was applied between the two boxes. The clear phase contrast in the two regions indicates the opposite ferroelectric FE polarizations in the CIPS controlled by the writing voltages.
Extended Data Fig. 6 The hysteric dependence of the tunnelling current of the F3GT/CIPS/F3GT MFTJ on the pulse writing voltage.
The tunnelling currents are measured by a −0.2 V d.c. reading voltage at room temperature after each attempted pulse writing voltage. The tunnelling currents show a square-shaped hysteresis loop as a dependence on the pulse writing voltages. Specifically, the pulse voltages of ±6 V switch the tunnelling currents in the MFTJ between ON and OFF states, confirming the FE switching of 2D CIPS and the non-volatile control of the tunnelling current.
Extended Data Fig. 7 FE hysteresis loops of a 44-nm-thick In2Se3 flake on a bulk F3GT flake.
The structure of this In2Se3/F3GT heterostructure is similar to the one in Extended Data Fig. 5a. Red and blue curves represent the out-of-plane PFM phase and amplitude as functions of the applied voltage between the PFM tip and the bottom Au electrode, respectively. FE hysteresis loops of the In2Se3 flake on the metallic F3GT flake show clear FE polarization switching under opposite applied electric voltages. The coercive voltage of the In2Se3 flake is ~2.5 V, which is consistent with the previous report55.
Extended Data Fig. 8 DFT calculated density of states (DOS) for F3GT/CIPS and F3GT/In2Se3 heterostructures under opposite FE polarizations.
a, DOS of monolayer F3GT (blue) and CIPS (red) under upward (up panel) and downward (bottom panel) FE polarizations. Fermi levels lie within the bandgap in both cases, indicating that the contacts between F3GT and CIPS are Schottky contacts under both FE polarizations. b, DOS of monolayer F3GT (blue) and In2Se3 (yellow) under upward (up panel) and downward (bottom panel) FE polarizations. Under the upward FE polarization, the contact between F3GT and In2Se3 is a Schottky contact, while the downward FE polarization forms an Ohmic contact between F3GT and In2Se3. Under the downward FE polarization, the zoomed-in inset of the bottom panel shows the calculated Fermi level located in the conduction band of In2Se3. Therefore, the ON-state current densities of F3GT/In2Se3/F3GT MFTJs are higher than those of F3GT/CIPS/F3GT MFTJs by a factor of 100 in our experimental results, possibly due to the reduced contact resistance between FE and FM materials when CIPS is replaced by In2Se3.
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Xie, T., Wang, Q., Zhang, H. et al. Tailorable multiferroic tunnel junctions from all-van der Waals multilayer stacking. Nat. Nanotechnol. (2026). https://doi.org/10.1038/s41565-025-02065-1
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DOI: https://doi.org/10.1038/s41565-025-02065-1
