# Fileset

[s41467-025-58224-4.pdf](https://mdr.nims.go.jp/filesets/6e96a917-0bc6-4699-835a-9ff3897b27e4/download)

## Creator

Shiming Huang, Lianying Zhu, Yongxin Zhao, [Kenji Watanabe](https://orcid.org/0000-0003-3701-8119), [Takashi Taniguchi](https://orcid.org/0000-0002-1467-3105), Jie Xiao, Le Wang, Jiawei Mei, Huolin Huang, Feng Zhang, Maoyuan Wang, Deyi Fu, Rong Zhang

## Rights

[Creative Commons BY-NC-ND Attribution-NonCommercial-NoDerivs 4.0 International](https://creativecommons.org/licenses/by-nc-nd/4.0/)

## Other metadata

[Giant magnetoresistance induced by spin-dependent orbital coupling in Fe3GeTe2/graphene heterostructures](https://mdr.nims.go.jp/datasets/516e5f46-b178-4d60-a1dd-b4e9d483d2e9)

## Fulltext

Giant magnetoresistance induced by spin-dependent orbital coupling in Fe3GeTe2/graphene heterostructuresArticle https://doi.org/10.1038/s41467-025-58224-4Giant magnetoresistance induced by spin-dependent orbital coupling in Fe3GeTe2/graphene heterostructuresShiming Huang 1, Lianying Zhu 1, Yongxin Zhao1, Kenji Watanabe 2,Takashi Taniguchi 2, Jie Xiao3, Le Wang 4, Jiawei Mei 3, Huolin Huang 5,Feng Zhang 1 , Maoyuan Wang 1 , Deyi Fu 1 & Rong Zhang 1Information technology has a great demand for magnetoresistance (MR)sensors with high sensitivity and wide-temperature-range operation. It is wellknown that space charge inhomogeneity in graphene (Gr) leads to finiteMR inits pristine form, and can be enhanced by increasing the degree of spatialdisorder. However, the enhanced MR usually diminishes drastically as thetemperature decreases. Here, by stacking a van der Waals ferromagnetFe3GeTe2 (FGT) on top of graphene to form an FGT/Gr heterostructure, wedemonstrate a positive MR of up to ~9400% under a magnetic field of 9 T atroom temperature (RT), an order of magnitude larger MR compared to puregraphene.More strikingly, the giantMRof the FGT/Grheterostructure sustainsover awide temperature range fromRTdown to 4K. Both control experimentsand DFT calculations show that the enhanced MR originates from spin-dependent orbital coupling between FGT and graphene, which is temperatureinsensitive. Our results open a new route for realizing high-sensitivity andwide-temperature-range MR sensors.MR is a fascinating magnetoelectric phenomenon that has attractedsignificant attention since decades ago due to its importance in bothfundamental science and practical applications1–7. Researchers aim todevelopMR sensorswith low energy consumption and high sensitivitythat can operate over a wide-temperature range. To achieve this, theMR of a variety of newcomer materials have been investigated in thepast, including Dirac and Weyl semimetals8–13, strange metals14–16, etc.The most notable feature of these materials is the widespread unsa-turated linear MR observed at cryogenic temperature. However, theMR usually maximizes at low temperature and decreases rapidly withincreasing temperature9–13, which greatly limits their practical applic-ability. As a two-dimensional (2D) Dirac semimetal, graphene has beenfound to show unsaturated linear MR caused by spatial chargeinhomogeneity inevitably seen in 2D systems at room temperature17–21,holding great promise for future applications.The MR of pristine graphene is finite, leaving a large room forimprovement. According to the effective medium theory22, the degreeof disorder or charge inhomogeneity in graphene directly affects itsMR. Therefore, various methods have been proposed to enhance theMR of monolayer graphene by increasing its disorder. For example,different nanoparticles, such as gold23, cobalt24 and nickel25, have beendecorated on the surface of graphene. But, the enhancement ofMRbysuch decoration method is not very effective. Alternative way tointroduce extra disorder into graphene is to place it on exotic sub-strates such as lattice-mismatched black phosphorous26, surface-terraced SrTiO327 and BiFeO3 nano-island array28. By doing so, theReceived: 6 September 2024Accepted: 14 March 2025Check for updates1Department of Physics, Engineering Research Center for Micro-Nano Optoelectronic Materials and Devices of Ministry of Education, Fujian Provincial KeyLaboratory of Semiconductor Materials and Applications, Xiamen University, Xiamen, China. 2National Institute for Materials Science, Tsukuba, Japan.3Department of Physics, Southern University of Science and Technology, Shenzhen, China. 4Shenzhen Institute for Quantum Science and Engineering,Southern University of Science and Technology, Shenzhen, China. 5School of Optoelectronic Engineering and Instrumentation Science, Dalian University ofTechnology, Dalian, China. e-mail: fzhang@xmu.edu.cn; mywang@xmu.edu.cn; dyfu@xmu.edu.cnNature Communications |         (2025) 16:2866 11234567890():,;1234567890():,;http://orcid.org/0009-0009-2455-3885http://orcid.org/0009-0009-2455-3885http://orcid.org/0009-0009-2455-3885http://orcid.org/0009-0009-2455-3885http://orcid.org/0009-0009-2455-3885http://orcid.org/0009-0008-5906-956Xhttp://orcid.org/0009-0008-5906-956Xhttp://orcid.org/0009-0008-5906-956Xhttp://orcid.org/0009-0008-5906-956Xhttp://orcid.org/0009-0008-5906-956Xhttp://orcid.org/0000-0003-3701-8119http://orcid.org/0000-0003-3701-8119http://orcid.org/0000-0003-3701-8119http://orcid.org/0000-0003-3701-8119http://orcid.org/0000-0003-3701-8119http://orcid.org/0000-0002-1467-3105http://orcid.org/0000-0002-1467-3105http://orcid.org/0000-0002-1467-3105http://orcid.org/0000-0002-1467-3105http://orcid.org/0000-0002-1467-3105http://orcid.org/0000-0002-1962-3510http://orcid.org/0000-0002-1962-3510http://orcid.org/0000-0002-1962-3510http://orcid.org/0000-0002-1962-3510http://orcid.org/0000-0002-1962-3510http://orcid.org/0000-0003-4933-4880http://orcid.org/0000-0003-4933-4880http://orcid.org/0000-0003-4933-4880http://orcid.org/0000-0003-4933-4880http://orcid.org/0000-0003-4933-4880http://orcid.org/0000-0003-4721-9459http://orcid.org/0000-0003-4721-9459http://orcid.org/0000-0003-4721-9459http://orcid.org/0000-0003-4721-9459http://orcid.org/0000-0003-4721-9459http://orcid.org/0000-0002-1163-2498http://orcid.org/0000-0002-1163-2498http://orcid.org/0000-0002-1163-2498http://orcid.org/0000-0002-1163-2498http://orcid.org/0000-0002-1163-2498http://orcid.org/0000-0001-7280-8947http://orcid.org/0000-0001-7280-8947http://orcid.org/0000-0001-7280-8947http://orcid.org/0000-0001-7280-8947http://orcid.org/0000-0001-7280-8947http://orcid.org/0000-0003-1365-8963http://orcid.org/0000-0003-1365-8963http://orcid.org/0000-0003-1365-8963http://orcid.org/0000-0003-1365-8963http://orcid.org/0000-0003-1365-8963http://orcid.org/0000-0003-0015-6331http://orcid.org/0000-0003-0015-6331http://orcid.org/0000-0003-0015-6331http://orcid.org/0000-0003-0015-6331http://orcid.org/0000-0003-0015-6331http://crossmark.crossref.org/dialog/?doi=10.1038/s41467-025-58224-4&domain=pdfhttp://crossmark.crossref.org/dialog/?doi=10.1038/s41467-025-58224-4&domain=pdfhttp://crossmark.crossref.org/dialog/?doi=10.1038/s41467-025-58224-4&domain=pdfhttp://crossmark.crossref.org/dialog/?doi=10.1038/s41467-025-58224-4&domain=pdfmailto:fzhang@xmu.edu.cnmailto:mywang@xmu.edu.cnmailto:dyfu@xmu.edu.cnwww.nature.com/naturecommunicationsroom-temperature MR has been enhanced significantly. However, theMR in these systems still shows severe temperature instability, whichcould be attributed to the highly temperature-dependent extrinsicdegree of disorder. Very recently, Dirac plasma has been generated ingraphene through sophisticated hexagonal boron nitride (h-BN)encapsulation technique, which achieves anMR as large as 110% under0.1 T and 8600% under 9 T at room temperature29. However, the Diracplasma only forms at the vicinity of Dirac point and sustains down toonly ~100K, which makes the MR decrease dramatically at low tem-perature as well as away from Dirac point.In order to achieve giant, stable MR in graphene in a broadertemperature range, alternative strategy with temperature insensitivityneeds to be introduced. Here, we propose a novel approach toenhance the MR of graphene by stacking the van der Waals ferro-magnet FGT on a monolayer graphene to form an FGT/Grheterostructure30,31. The FGT/Gr heterostructure can achieve a MR ofup to ~9400% under 9 T at room temperature away from Dirac point,which is more than thirty-fold enhancement over the MR of puregraphene. More importantly, the giant MR sustains in the full tem-perature range studied from RT down to 4K and even slightlyincreases with lowering temperature. DFT calculations show that whenFGT is placed on graphene, the magnetism of FGT breaks the spin-degeneracy of graphene, where the spin majority carriers with lowmobility contribute little conductivity while the spin minority carrierswith highmobility dominates in transport. When an external magneticfield is applied, the density of spin minority carriers decreases rapidly,resulting in the reduction of conductivity and thus giantMR. Our worksheds light on the development of next generation MR sensors andrelevant spintronic devices with high sensitivity and wide working-temperature range.Results and discussionGiant MR at room temperatureWe fabricated the FGT/Gr heterostructure device by using a simple drytransfer method followed by standard electron-beam lithography andmetal deposition procedure (seeMethods for details). A typical device(Device A) is shown in Fig. 1a, where Hall-bar shaped electrodes arepatterned directly on graphene ribbon, dividing the channel into twoparts: pure graphene region and FGT/Gr heterostructure region. TheMR for both regions were measured by recording the longitudinalresistanceRxx as a function of perpendicularly appliedmagnetic field Bin a four-probe geometry and calculated as MR= (Rxx(B)-Rxx(0))/Rxx(0) × 100%, where Rxx(B) and Rxx(0) are the resistance values atfinite field and zero field, respectively.The four-probe current-voltage (I–V) curves across the FGT/Grheterostructure region under different magnetic fields were firstmeasured and shown in Fig. 1b. As can be seen, the inverse slope of theI–V curves, which corresponds to the longitudinal resistance Rxx,Fig. 1 | Device structure and basic magneto-transport measurements at roomtemperature. a Optical microscope image of a typical FGT/Gr heterostructuredevice (Device A) and schematic illustration ofmeasurement setup. The reddashedline in the photograph indicates the monolayer graphene. Scale bar is 10 µm. b I–Vcurves of the FGT/Gr heterostructure in Device A under different magnetic fields.c Room-temperatureMR of the FGT/Gr heterostructure in Device A as a function ofmagnetic field. The MR curve of the pure graphene region is also shown for com-parison. dHall resistances Rxy of the FGT shown in the inset as a function of out-of-plane magnetic field at various temperatures ranging from 1.6 to 225K. Scalebar is 5 µm.Article https://doi.org/10.1038/s41467-025-58224-4Nature Communications |         (2025) 16:2866 2www.nature.com/naturecommunicationschanges dramatically with increasing magnetic field, pointing to alarge MR. Next, by scanning the magnetic field continuously under aconstant sourcing current, theMR curves of both the graphene regionand the FGT/Gr heterostructure region weremeasured, calculated andplotted in Fig. 1c. The MR of the FGT/Gr heterostructure reaches~9400% under 9 T at room temperature, while that of the pure gra-phene is less than 300% which is comparable to previous reportedvalues19,21. Themore than thirty-fold enhancement ofMR inour FGT/Grheterostructure is appreciable and to the best of our knowledge, theabsolute value sets a record as compared to previous reports on dif-ferent graphene-based systems (refer to Fig. 4c and SupplementaryTable 1)8,19–21,23–29.The origin of the giantMR fromFGT itself has to be ruled out first.The magneto-transport properties of FGT with comparable thickness(~40 nm) to that of the one used in Device A were characterized bymaking a Hall bar device as shown in the inset of Fig. 1d. The anom-alous Hall effect measurement shows that the Curie temperature (Tc)of the van der Waals ferromagnet FGT is ~210K with an out-of-planeeasy axis32. The MR curves of the FGT both below and above Tc weremeasured in the same way as aforementioned and shown in Supple-mentary Fig. 1. The negligibly small MR agrees with previous report33,indicating that the FGT alone cannot contribute to the giant MRobserved in our FGT/Gr heterostructure.Temperature, angle and gate-dependence of MRThe MR curves at different temperatures in Device A were measuredand shown in Fig. 2a. We note that the oscillatory and negative MRusually seen at cryogenic temperature in pure graphene (Supplemen-tary Fig. 5) and other graphene based heterostructures is absent in oursystem. Instead, theMR increasesmonotonically withmagneticfield inthe whole temperature range studied. These features suggest that theweak (anti)localization and universal conductance fluctuation aresuppressed in our system26,27. The temperature-dependent MR underfixed magnetic fields were further plotted in Fig. 2b. Strikingly, thegiantMRobserved at room temperature stays almost unchangedwhentemperature decreases, in stark contrast to the trend observed inpreviously studied graphene-based systems8,19,20,23,26,29, which impliesthat the giant MR in our FGT/Gr heterostructure may have a differentorigin. We emphasize that such temperature-insensitive MR favorsmagnetic sensor applications at both room temperature and cryogenictemperature regimes. Next, the angular dependence of the Rxx onmagnetic field direction was routinely checked and shown in Supple-mentary Figs. 2 and 5. The Rxx is at its maximum (minimum) when themagnetic field is perpendicular (parallel) to the sample surface, fol-lowing a cosine dependence. Therefore, our FGT/Gr heterostructurecomplies with the classical MR mechanism, where the Lorentz forcetakes effect34.Figure 2c shows the transfer curves of another device (Device C)under different magnetic fields. As can be seen, the Dirac point ofgraphene in the FGT/Gr heterostructure is at −2.5 V under zero mag-netic field and remains almost unchanged up to high magnetic fields.The gate-voltage-dependent MR was calculated from Fig. 2c andplotted in Fig. 2d for three representative magnetic fields. Similar toprevious reports19,23,26,29, the MR is maximized around the Dirac pointFig. 2 | Temperature- and gate-dependentMRof FGT/Gr heterostructure. a TheMR curves of FGT/Gr heterostructure in Device A as a function of magnetic field atdifferent temperature points. b Variation of MR with temperature under differentmagneticfields inDeviceA. cTransfer curves of FGT/Gr heterostructure inDeviceCmeasured at room temperature under different magnetic fields. d Normalized MRof the FGT/Gr heterostructure in Device C under three representative magneticfields as a function of gate voltage.Article https://doi.org/10.1038/s41467-025-58224-4Nature Communications |         (2025) 16:2866 3www.nature.com/naturecommunicationsand decreases gradually away from it. It is noted that theMRdecreasesfaster under low field while slower under high field.Understanding the origin of the giant MRIt is unclear why FGT, a ferromagnet with minimal MR on their own(less than 1% under 9 T), can increase the latter’s MR by more than anorder of magnitude when formed into heterostructures with mono-layer graphene. To understand the physical mechanism inside, weperformed a density functional theory (DFT)35,36 calculation of FGT onmonolayer graphene, as shown schematically in Fig. 3a. The spinresolution band structures projected to graphene and FGT are plottedin Fig. 3b, c, respectively. It can be seen from Fig. 3b that around Fermienergy (−0.08 eV), the spin-down bands (blue bands) of graphene arecoupledwith the spin-downbandsof FGT,while the spin-upbands (redbands) of graphene almost keep its original linear dispersion, due tothe lack of spin-up bands of FGT around the Fermi level, leading tostrong hybridization of only one spin channel. Similar phenomenonhas been reported in graphene proximitized by ferromagnetic insu-lator CrI3 recently37. Here, we regard spin-down with larger density ofstates (DOS) at Fermi level as majority spin and spin-up with smallerDOS at Fermi level asminority spin. Aswell known, the highmobility ofgraphene originates from its linear dispersion and pseudo-spin ofDirac cone. Therefore, the breaking of the linear dispersion of gra-phene spin-down bands makes the majority spin carriers scattered byFGT easily, resulting inmuch lowermobility ofmajority spin carriers ascompared with that ofminority spin carriers. The total conductivity ofgraphene proximitized by FGT can be written as: σB = e n"μ" +n#μ#� �,where n"=# and μ"=# are the density and mobility of spin-up/downcarriers, respectively. When there is nomagnetic field, we have n" <n#and μ" ≫μ# as aforementioned, therefore the conductivity of gra-phene σB=0 � en"μ". When an external magnetic field B is applied, thespin-down bands move downward, with larger DOS, while the spin-upbands move upward, with smaller DOS. Based on conservation ofparticle number, n" +n# +NFGT,# =Const:, we haveδn" =δn# +δNFGT,# δn � n Bð Þ � n B=0ð Þ�� ��� �, which means that thedensity of spin-up (minority) carriersn" reducesmuch faster than spin-down (majority) carriers n# increases, resulting in rapid reduction ofthe conductivity of graphene σB � en"ðBÞμ" and therefore thegiant MR.To demonstrate the uniqueness of FGT on the enhancement ofthe MR in graphene, we stacked CrGeTe3 (CGT)38, a 2D ferromagneticsemiconductor, on monolayer graphene to make a CGT/Gr hetero-structure device. The device image and measurement results are pre-sented in Supplementary Fig. 8. It is found that there is no MRenhancement at all and the MR of the heterostructure even decreasesas compared to the pure graphene. DFT calculations on the CGT/Grheterostructure were also performed and the results are shown inSupplementary Fig. 9. Different from the FGT/Gr case, the energy bandhybridization between CGT and graphene is inappreciable, thereforespin-dependant orbital coupling induced MR enhancement effect isnot expected as shown in Supplementary Fig. 8. Likewise, we alsostacked MoS2, a 2D nonmagnetic semiconductor, with monolayergraphene to make a MoS2/Gr heterostructure device. The measure-ment results presented in Supplementary Fig. 10 also show negligibleMR enhancement effect. The MR obtained from different hetero-structures in our work are summarized in Fig. 4a, where only FGT/Grshows giant MR as compared to others, pointing to the unique role ofFGT on enhancing the MR in graphene as aforementioned.We also note that vacuum annealing can help to improve thecoupling between FGT and graphene, therefore enhance theMRof theheterostructure. It is a common way to do vacuum annealing in orderto enhance the interfacial coupling in van der Waals heterostructuresFig. 3 | Theoretical calculation. a Crystal structure of FGT/Gr heterostructure. b The spin-resolution band structure, projected to graphene. c The spin-resolution bandstructure, projected to FGT. The dashed lines in both (b, c) indicate the Fermi level.Fig. 4 | Statistics ofMR indifferent devices. aHistogramofMRunder 1 Tmagneticfield fordifferent structures studied in thiswork.bVariation ofMRunder 9 Tmagneticfield with annealing temperature for different groups of devices. c Comparison of MR for different graphene-based systems reported in our work and literatures.Article https://doi.org/10.1038/s41467-025-58224-4Nature Communications |         (2025) 16:2866 4www.nature.com/naturecommunicationsby driving out the trapped air/moisture asmuch as possible39–42, whichdepends on the annealing temperature and time. As shown in Fig. 4band Supplementary Fig. 4c, the as-fabricated FGT/Gr heterostructureshows MR of only ~300% under 9 T (Device C), which is neverthelessstill higher than that of pure graphene. After annealing in high vacuumat 170 °C (see Methods), the MR of the heterostructure drasticallyincreased to ~760%. For devices with even higher annealing tempera-ture (220 °C and 250 °C), the MR all reached above ~2000% withhighest value of ~9400%. For pure graphene and other hetero-structures studied in this work, however, vacuum annealing showedlittle enhancement of the MR. This further supports that the giant MRin FGT/Gr heterostructure originates from the unique interfacial cou-pling induced spin-split band hybridization between FGT and gra-phene, rather than other artificial effects.In summary, giant MR of up to ~9400% under 9 T at room tem-perature has been observed in FGT/Gr heterostructure, in which themore than one order of magnitude enhancement of MR as comparedto pure graphene originates from spin-dependent orbital couplingbetween FGT and graphene. While in graphene heterostructuresformed with either ferromagnetic semiconductor CGT or non-ferromagnetic semiconductor MoS2, such spin-dependent coupling isnegligible, leading to little MR enhancement. Strong spin-dependenthybridization was recently predicted in CrI3/Gr heterostructure37,therefore similar MR enhancement effect may also exist, which needsto be further studied. More importantly, the giant MR of FGT/Gr het-erostructure at room temperature stays almost unchanged withdecreasing temperature, which is strikingly different from thetemperature-dependent behavior in previously reported systems.With rapid advancement of growing large-area graphene and related2D materials, our work holds an attractive prospect for fabricatinghighly sensitive graphene-based magnetic sensors with wide tem-perature operation ranges.MethodsHeterostructure preparation and device fabricationMonolayer graphene was prepared by mechanically peeling high-quality graphite (natural graphite from HQ Graphene) ontoSiO2(285 nm)/Si substrate and identified by optical contrast as well asRaman spectra. Multilayer Fe3GeTe2 was exfoliated and transferredonto monolayer graphene by PDMS dry transfer technique in glovebox (O2, H2O< 1 ppm). Electrodes were patterned by e-beam litho-graphy and then Ti/Au (2 nm/50 nm) was deposited by an e-beamevaporator with base pressure of 10−7Torr. Standard lift-off procedurewas done subsequently and blowed dry with Ar gun. Finally, multilayerh-BN was exfoliated and transferred onto the device channel region toprevent Fe3GeTe2 from being oxidized in air. For CGT/Gr andMoS2/Grheterostructure devices, same procedures were followed. For vacuumannealing, device was put into a tube furnace equipped with turbopump station (base pressure: 10−6Torr) and kept at different tem-peratures for 3 h.Magneto-transport measurementsThe magneto-transport measurements were carried out in a Cryofreesuperconducting magnet system (CFMS-12T-30VTI, Cryogenic Co.)withmagneticfield up to 12 T by using two sourcemeters (Model 2400andModel 2450, Keithley Inc.). To apply back gate voltage, the sourceterminal was connected to the back gate and the leakage currentthrough the SiO2 dielectric layer was monitored.Theoretical calculation detailsThe first-principles calculations were performed using Vienna ab initiosimulation package (VASP) based on the density function theory withLDA+U. The energy cut off of the plane wave basis was set as 400 eV,and the Brillouin zone was sampled by 6 × 6 × 1 k-mesh.Data availabilityThe source data generated in this study have been deposited in thefigshare database under accession code43.References1. Baibich, M. N. et al. Giant magnetoresistance of (001)Fe/(001)Crmagnetic superlattices. Phys. Rev. Lett. 61, 2472–2475 (1988).2. Abrikosov, A. A.Quantum linearmagnetoresistance. Europhys. Lett.49, 789–793 (2000).3. Parish, M. M. & Littlewood, P. B. Non-saturating magnetoresistancein heavily disordered semiconductors.Nature 426, 162–165 (2003).4. Parkin, S. S. P. et al. Giant tunnelling magnetoresistance at roomtemperature with MgO (100) tunnel barriers. Nat. Mater. 3,862–867 (2004).5. Ripka, P. & Janosek, M. Advances in magnetic field sensors. IEEESens. J. 10, 1108–1116 (2010).6. Friedman, A. L. et al. Quantum linear magnetoresistance in multi-layer epitaxial graphene. Nano Lett. 10, 3962–3965 (2010).7. Fang, J. Z. et al. Large unsaturated magnetoresistance of 2D mag-netic semiconductor Fe-SnS2 homojunction. J. Semicond. 43,092501 (2022).8. Cho, S. & Fuhrer, M. S. Charge transport and inhomogeneity nearthe minimum conductivity point in graphene. Phys. Rev. B 77,081402(R) (2008).9. Ali, M. N. et al. Large, non-saturating magnetoresistance in WTe2.Nature 514, 205–208 (2014).10. Liang, T. et al. Ultrahighmobility andgiantmagnetoresistance in theDirac semimetal Cd3As2. Nat. Mater. 14, 280–284 (2015).11. Thoutam, L. R. et al. Temperature-dependent three-dimensionalanisotropy of the magnetoresistance in WTe2. Phys. Rev. Lett. 115,046602 (2015).12. Shekhar, C. et al. Extremely large magnetoresistance and ultrahighmobility in the topological Weyl semimetal candidate NbP. Nat.Phys. 11, 645–649 (2015).13. Kumar, N. et al. Extremely high magnetoresistance and con-ductivity in the type-II Weyl semimetals WP2 and MoP2. Nat. Com-mun. 8, 1642 (2017).14. Phillips, P. W., Hussey, N. E. & Abbamonte, P. Stranger than metals.Science 377, eabh4273 (2022).15. Hayes, I. et al. Scaling between magnetic field and temperature inthe high-temperature superconductor BaFe2(As1−xPx)2. Nat. Phys.12, 916–919 (2016).16. Giraldo-Gallo, P. et al. Scale-invariant magnetoresistance in a cup-rate superconductor. Science 361, 479–481 (2018).17. Novoselov, K. S. et al. Two-dimensional gas of massless Dirac fer-mions in graphene. Nature 438, 197–200 (2005).18. Castro Neto, A. H., Guinea, F., Peres, N. M. R., Novoselov, K. S. &Geim, A. K. The electronic properties of graphene. Rev. Mod. Phys.81, 109–162 (2009).19. Gopinadhan, K., Shin, Y. J., Yudhistira, I., Niu, J. & Yang, Y. Giantmagnetoresistance in single-layer graphene flakes with a gate-voltage-tunable weak localization. Phys. Rev. B 88, 195429 (2013).20. Chuang, C. S., Yang, Y. F., Elmquist, R. E. & Liang, C.-T. Linearmagnetoresistance in monolayer epitaxial graphene grown on SiC.Mater. Lett. 174, 118–121 (2016).21. Chuang, C. S. et al. Large, non-saturating magnetoresistance insingle layer chemical vapor deposition graphene with an h-BNcapping layer. Carbon 136, 211–216 (2018).22. Tiwari, R. P. & Stroud, D. Model for the magnetoresistance and Hallcoefficient of inhomogeneous graphene. Phys. Rev. B 79,165408 (2009).23. Jia, Z. Z. et al. Large tunable linear magnetoresistance in goldnanoparticle decorated graphene. Appl. Phys. Lett. 105,143103 (2014).Article https://doi.org/10.1038/s41467-025-58224-4Nature Communications |         (2025) 16:2866 5www.nature.com/naturecommunications24. Wang, Q. et al. Enhanced room-temperature positive magnetore-sistance of graphene by decorating Co particles on the surface.Mater. Lett. 293, 129730 (2021).25. Cruz, E. A., Ducos, P., Gao, Z., Johnson, A. T. C. & Niebieskikwiat, T.Exchange coupling effects on the magnetotransport properties ofNi-nanoparticle-decorated graphene. Nanomaterials 13,1861 (2023).26. Liu, Y. P. et al. Phonon-mediated colossal magnetoresistance ingraphene/black phosphorus heterostructures. Nano Lett. 18,3377 (2018).27. Hu, J. X. et al. Room-temperature colossal magnetoresistance interraced single-layer graphene. Adv. Mater. 32, 2002201 (2020).28. Jeon, J. et al. Large temperature-independent magnetoresistancewithout gating operation in monolayer graphene. ACS Appl. Mater.Interfaces 12, 53134 (2020).29. Xin, N. et al. Giant magnetoresistance of Dirac plasma in high-mobility graphene. Nature 616, 270–274 (2023).30. Deng, Y. et al. Gate-tunable room-temperature ferromagnetism intwo-dimensional Fe3GeTe2. Nature 563, 94–99 (2018).31. Gibertini, M., Koperski, M., Morpurgo, A. F. & Novoselov, K. S.Magnetic 2D materials and heterostructures. Nat. Nanotechnol. 14,408–419 (2019).32. Feng, H. et al. Resistance anomaly and linear magnetoresistance inthin flakes of itinerant ferromagnet Fe3GeTe2. Chin. Phys. Lett. 39,077501 (2022).33. Zeng, X. et al. Magnetoresistance studies of two-dimensionalFe3GeTe2 nano-flake. J. Phys.: Condens. Matter 34, 345701 (2022).34. Gopinadhan, K. et al. Extremely large magnetoresistance in few-layer graphene/boron–nitride heterostructures. Nat. Commun. 6,8337 (2015).35. Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initiototal-energy calculations using a plane-wave basis set. Phys. Rev. B54, 11169 (1996).36. Kresse, G. & Joubert, D. From ultrasoft pseudopotentials to theprojector augmented-wave method. Phys. Rev. B 59,1758–1775 (1999).37. Cardoso, C., Costa, A. T., MacDonald, A. H. & Fernández-Rossier, J.Strongmagnetic proximity effect in van derWaals heterostructuresdriven by direct hybridization. Phys. Rev. B 108, 184423 (2023).38. Li, X. X. &Yang, J. L. CrXTe3 (X =Si, Ge) nanosheets: twodimensionalintrinsic ferromagnetic semiconductors. J. Mater. Chem. C. 2,7071–7076 (2014).39. Diaz, H.C., Addou, R. &Batzill, M. Interfaceproperties ofCVDgrowngraphene transferred onto MoS2(0001). Nanoscale 6,1071–1078 (2014).40. Wang, K. et al. Interlayer coupling in twisted WSe2/WS2 bilayerheterostructures revealed by optical spectroscopy. ACS Nano 10,6612–6622 (2016).41. Yue, X. et al. Monitoring and engineering interface couplingbetween monolayer WS2 and substrate through controllably intro-ducing interfacial strain. Sci. China Mater. 67, 3012–3020 (2024).42. Tang, L. et al. Enhancing magnetocrystalline anisotropy throughinterface coupling in a 2D ferromagnetic Fe3GeTe2/VI3 hetero-structure. Appl. Phys. Lett. 124, 012403 (2024).43. Huang, S. et al. Giant magnetoresistance induced by spin-dependent orbital coupling in Fe3GeTe2/graphene hetero-structures. figshare. Dataset. https://doi.org/10.6084/m9.figshare.28539461 (2025).AcknowledgementsD.F. acknowledges support by the National Natural Science Foundation ofChina (No. 62174143) and the Fundamental Research Funds for theCentral Universities (No. ZK1245). M.W. acknowledges support by theNatural Science Foundation of Xiamen, China (No. 3502Z202472008).F.Z. acknowledges support by the National Natural Science Foundation ofChina (Nos. 62274137 and 62104222), Natural Science Foundation ofJiangxi Province of China for Distinguished Young Scholars (No.S2021QNZD2L0013) and National Key Research and Development Pro-gram of China (No. 2023YFB3609500). J.X., L.W. and J.M. acknowledgesupport by theNational Key Research andDevelopment ProgramofChina(No. 2021YFA1400400) and the Shenzhen Fundamental Research Pro-gram (Nos. JCYJ20220818100405013 and JCYJ20230807093204010).H.H. acknowledges support by the Science and Technology InnovationFund of Dalian (No. 2022JJ12GX011).Author contributionsD.F. and R.Z. initiated, coordinated, and supervised the work. S.H., L.Z.and Y.Z. fabricated the devices. S.H. performed the measurements.M.W. did the theoretical calculations. J.X., L.W. and J.M. grew theFe3GeTe2 crystals. K.W. and T.T. grew the h-BN crystals. S.H., F.Z., M.W.and D.F. participated in the data analysis and manuscript writing.Competing interestsThe authors declare no competing interests.Additional informationSupplementary information The online version containssupplementary material available athttps://doi.org/10.1038/s41467-025-58224-4.Correspondence and requests for materials should be addressed toFeng Zhang, Maoyuan Wang or Deyi Fu.Peer review informationNature Communications thanks Jung-Woo Yooand the other, anonymous, reviewer(s) for their contribution to the peerreview of this work. A peer review file is available.Reprints and permissions information is available athttp://www.nature.com/reprintsPublisher’s note Springer Nature remains neutral with regard tojurisdictional claims in published maps and institutional affiliations.Open Access This article is licensed under a Creative CommonsAttribution-NonCommercial-NoDerivatives 4.0 International License,which permits any non-commercial use, sharing, distribution andreproduction in any medium or format, as long as you give appropriatecredit to the original author(s) and the source, provide a link to theCreative Commons licence, and indicate if you modified the licensedmaterial. Youdonot havepermissionunder this licence toshare adaptedmaterial derived from this article or parts of it. The images or other thirdparty material in this article are included in the article’s CreativeCommons licence, unless indicated otherwise in a credit line to thematerial. If material is not included in the article’s Creative Commonslicence and your intended use is not permitted by statutory regulation orexceeds the permitted use, you will need to obtain permission directlyfrom the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.© The Author(s) 2025Article https://doi.org/10.1038/s41467-025-58224-4Nature Communications |         (2025) 16:2866 6https://doi.org/10.6084/m9.figshare.28539461https://doi.org/10.6084/m9.figshare.28539461https://doi.org/10.1038/s41467-025-58224-4http://www.nature.com/reprintshttp://creativecommons.org/licenses/by-nc-nd/4.0/http://creativecommons.org/licenses/by-nc-nd/4.0/www.nature.com/naturecommunications Giant magnetoresistance induced by spin-dependent orbital coupling in Fe3GeTe2/graphene heterostructures Results and discussion Giant MR at room temperature Temperature, angle and gate-dependence of MR Understanding the origin of the giant MR Methods Heterostructure preparation and device fabrication Magneto-transport measurements Theoretical calculation details Data availability References Acknowledgements Author contributions Competing interests Additional information