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Jinhyoung Lee, Gunhyoung Kim, Hyunho Seok, Hyunbin Choi, Hyeonjeong Lee, Seokchan Lee, Geonwook Kim, Hyunho Kim, Seowoo Son, Sihoon Son, Dongho Lee, Hosin Hwang, Hyelim Shin, Sujeong Han, Geumji Back, Alexina Ollier, Yeon‐Ji Kim, Lei Fang, Gyuho Han, Goo‐Eun Jung, Youngi Lee, Hyeong‐U Kim, [Kenji Watanabe](https://orcid.org/0000-0003-3701-8119), [Takashi Taniguchi](https://orcid.org/0000-0002-1467-3105), Wonjun Shin, Suraj Cheema, Andreas Heinrich, Won‐Jun Jang, Taesung Kim

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[Artificial Room‐Temperature Ferromagnetism of Bulk van der Waals VSe<sub>2</sub>](https://mdr.nims.go.jp/datasets/de5a900b-a70a-421d-a76f-50b19d29f472)

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Artificial Room‐Temperature Ferromagnetism of Bulk van der Waals VSe2RESEARCH ARTICLEwww.advancedscience.comArtificial Room-Temperature Ferromagnetism of Bulk vander Waals VSe2Jinhyoung Lee, Gunhyoung Kim, Hyunho Seok, Hyunbin Choi, Hyeonjeong Lee,Seokchan Lee, Geonwook Kim, Hyunho Kim, Seowoo Son, Sihoon Son, Dongho Lee,Hosin Hwang, Hyelim Shin, Sujeong Han, Geumji Back, Alexina Ollier, Yeon-Ji Kim,Lei Fang, Gyuho Han, Goo-Eun Jung, Youngi Lee, Hyeong-U Kim, Kenji Watanabe,Takashi Taniguchi, Wonjun Shin, Suraj Cheema, Andreas Heinrich, Won-Jun Jang,and Taesung Kim*Originating from spin and orbital motion, van der Waals (vdW) ferromagnetismhas emerged as a significant platform to experimentally accessthe fundamental physics of magnetism in reduced dimensions, includingquantum computing, sensing, and data storage. However, currently, availablevdW ferromagnetic materials can be achieved with mechanical exfoliation andlow-temperature operation, which completely limits the monolithic integrationof vdW ferromagnets with other functional materials. Nonetheless, the directsynthesis of room-temperature vdW ferromagnets has not been achievedcommercially, owing to the imprecise control of the layer-by-layer growth,high-temperature synthesis, and low yield. To overcome these limitations,herein, an artificial vdW ferromagnetic platform has been reported, whichactivates the nano-crystallization and its corresponding ferromagnetismin bulk VSe2 via Ar + H2S plasma sulfurization. Sweeping the magneticfield, vdW ferromagnetism has been spatially resolved, which experimentallycorrelates with magnetization reversal behavior and domain pinning effects.Furthermore, nano-crystallization of VSe2 is clearly validated with transmissionelectronmicroscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectronspectroscopy, and selected area diffraction analysis. In conclusion, it isenvisioned that the artificial vdW ferromagnetic platform can artificially injectthe ferromagnetism in bulk vdW VSe2, which has not been possible previously.J. Lee, H. Lee, G. Kim, D. Lee, T. KimSchool of Mechanical EngineeringSungkyunkwan University (SKKU)Suwon-si, Gyeonggi-do 16419, South KoreaE-mail: tkim@skku.eduThe ORCID identification number(s) for the author(s) of this articlecan be found under https://doi.org/10.1002/advs.202504746© 2025 The Author(s). Advanced Science published by Wiley-VCHGmbH. This is an open access article under the terms of the CreativeCommons Attribution License, which permits use, distribution andreproduction in any medium, provided the original work is properly cited.DOI: 10.1002/advs.2025047461. IntroductionFor centuries, the enigmatic properties oflodestones and their magnetic attraction toiron, as well as the remarkable navigationalabilities of birds, fish, and insects acrossvast distances, have captivated human cu-riosity. Prior to the advent of electromag-netism and quantum mechanics, it was in-conceivable that these phenomena mightshare a common magnetic foundation.[1]Magnetism, which is as pervasive as theelectron itself, fundamentally originatedfrom the motion and spin of elementaryparticles. Its applications span living organ-isms, energy harvesting, data storage, andmedical diagnostics. When the microscopic“electron magnets” align spontaneously,magnetic order emerges as a fundamentalphase of matter, enabling the developmentof functional devices such as electric gen-erators, motors, magneto-resistive memo-ries, and optical isolators. The electron,often regarded as a minute magnet withtwo opposing poles, generates a magneticfield through its spin and orbital motion.J. Lee, A. Ollier, Y.-J. Kim, L. Fang, A. Heinrich, W.-J. JangCenter for Quantum NanoscienceInstitute for Basic Science (IBS)Seoul 03760, South KoreaG. Kim, H. Choi, H. Kim, H. Hwang, H. Shin, S. Han, G. Back, W. Shin,T. KimDepartment of Semiconductor Convergence EngineeringSungkyunkwan UniversitySuwon 16419, South KoreaH. Seok, S. Lee, S. Son, S. Son, T. KimSKKU Advanced Institute of Nanotechnology (SAINT)Sungkyunkwan UniversitySuwon 16419, South KoreaH. Seok, S. Lee, S. Son, S. Son, T. KimDepartment of Nano Science and TechnologySungkyunkwan UniversitySuwon 16419, South KoreaAdv. Sci. 2025, 12, e04746 e04746 (1 of 9) © 2025 The Author(s). Advanced Science published by Wiley-VCH GmbHhttp://www.advancedscience.commailto:tkim@skku.eduhttps://doi.org/10.1002/advs.202504746http://creativecommons.org/licenses/by/4.0/http://creativecommons.org/licenses/by/4.0/http://crossmark.crossref.org/dialog/?doi=10.1002%2Fadvs.202504746&domain=pdf&date_stamp=2025-05-30www.advancedsciencenews.com www.advancedscience.comThe collective alignment of these microscopic magnets, drivenby intrinsic coupling, raises the emergence of ferromagnetism.[2]However, the Mermin-Wagner theorem[3] suggested that ferro-magnetism cannot be persisted in two-dimensional (2D) van derWaals (vdW) systems owing to its thermal fluctuations.Recent breakthroughs in vdW magnetic crystals have demon-strated that magnetic anisotropy can stabilize long-range mag-netic order by creating an excitation gap that counteracts ther-mal agitation.[4] vdW magnetic crystals serve as ideal plat-forms for exploring magnetism in reduced dimensions,[5] of-fering advantages over traditional magnetic thin films. Thesematerials are largely decoupled from substrates,[6] electricallytunable,[7] mechanically flexible,[8] and amenable to chemicalfunctionalization.[9] In early 2017, the first evidence of long-range magnetic order in pristine vdW crystals was reported inCr2Ge2Te6[10] and CrI3,[11] both magnetic insulators with dis-tinct properties. Conversely, vdW Fe3GeTe2[12] was identified as amagnetic conductor, highlighting the diverse applications of itin-erant magnets [13] and magnetic insulators.[14] Advances in ma-nipulating individual vdW layers have enabled the fabrication ofmultilayer “designer magnets” [15] with notable outcomes suchas giant cross-layer tunneling magnetoresistance [16] throughengineered interlayer magnetic coupling. In heterostructurescombining electronic and photonic materials, the integrationG. Han, G.-E. Jung, Y. LeePark Systems Corporation109, Gwanggyo-ro, Yeongtong-gu, Suwon-si, Gyeonggi-do 16229, SouthKoreaH.-U KimSemiconductor Manufacturing Research CenterKorea Institute of Machinery and Materials (KIMM)Daejeon 34103, South KoreaH.-U KimNano-MechatronicsKIMM CampusUniversity of Science & Technology (UST)Daejeon 34113, South KoreaK. Watanabe, T. TaniguchiNational Institute for Materials ScienceNamiki 1-1Tsukuba, Ibaraki 305-0044, JapanH. Seok, S. CheemaResearch Laboratory of ElectronicsMassachusetts Institute of TechnologyCambridge, MA 02139, USAS. CheemaDepartment of Electrical Engineering and Computer ScienceMassachusetts Institute of TechnologyCambridge, MA 02139, USAH. Seok, S. CheemaDepartment of Materials Science and EngineeringMassachusetts Institute of TechnologyCambridge, MA 02139, USAA. Ollier, A. Heinrich, W.-J. JangDepartment of PhysicsEwha Womans UniversitySeoul 03760, South KoreaT. KimDepartment of Nano EngineeringSungkyunkwan UniversitySuwon 16419, South Koreaof distinct physical properties can lead to versatile functionali-ties, including heterostructuremultiferroicity,[17] unconventionalsuperconductivity,[18] and the quantum anomalousHall effect.[19]Major limitations of vdW ferromagnetic heterostructure corre-spond to the precise kinetic control of stacking order [20] andlarge-scale control over layer thickness [21] and crystallinity.[22]To address these challenges, researchers have focused onthe extrinsic methods to artificially induce magnetism in non-ferromagnetic vdW crystals. These approaches include i) defectengineering through vacancies, adatoms, grain boundaries, oredges; [23] ii) substitution of magnetic species; [24] and iii) themagnetic proximity effect,[25] where vdWmaterials are interfacedwith magnetic substrates. However, establishing long-range cor-relations between extrinsically introducedmagneticmoments re-mains difficult, and substrate-inducedmagnetic responses are of-ten limited. Theoretical proposals for inducing ferromagnetismby modifying lattice and band structures have yet to be experi-mentally realized, arising from the intrinsic vdW lattice struc-ture. In contrast, when ferromagnetism originating from itsvdW lattice structure can be experimentally realized, it will drivethe versatile advances for vdW ferromagnets [2] and their corre-sponding applications for electronic,[26] spintronics,[27] and next-generation quantum devices.[28] These underlying limitations ofthe conventional vdW ferromagnets motivated us to develop anon-demand synthesis method of vdW ferromagnet.Herein, we report an artificial vdW ferromagnetic platform fornon-magnetic vdW crystals, which provides a systematic solutionfor conventional vdW ferromagnets. To artificially activate the fer-romagnetism in bulk vdW VSe2, lattice distortion has been con-ducted with Ar + H2S plasma sulfurization, which correspondsto the ion penning effects and ion penetration. The artificial vdWferroelectricity activates the ferromagnetic manipulation regard-less of the number of vdW layers, which comprehensively over-comes the limitations of conventional vdW ferromagnetism. Ar-tificial vdW ferromagnetism was locally observed with MagneticForce Microscopy (MFM) imaging. The MFM junction was con-structed using a Co-coated magnetic tip, magnetically shieldedsample holder, and dual-permanent-magnet generator capableof sweeping the in-plane magnetic field from -500 to +500 Oe.The spatial resolution of magnetic domains was achieved by de-coupling topography and magnetic force measurements at con-trolled tip-sample distances (5 and 25 nm, respectively). [[ Accord-ing to the direction of the magnetic field of the MFM junction,vdW ferromagnetism has been spatially resolved with local fer-romagnetic domain mapping of nano-crystallized VSe2, whichexperimentally correlates with magnetization reversal behaviorand domain pinning effects. Furthermore, nano-crystallization ofVSe2 was clearly validated with atomic force microscopy (AFM),transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS),selected area diffraction (SAED) and Raman spectra measure-ments. In conclusion, we envision that our artificial vdW fer-romagnetic platform can artificially manipulate the ferromag-netism in bulk vdW VSe2 via nano-crystallization, which hasnot been possible previously. Unlike previously reported intrin-sic room-temperature vdW ferromagnets such as Cr1+xTe2,[31]Fe5GeTe2[32] and Fe3GaTe2,[33] which rely on definedmagnetic or-dering. Nevertheless, critical challenges persist, including intri-cate magnetic interactions across atomic lattices, scalability limi-Adv. Sci. 2025, 12, e04746 e04746 (2 of 9) © 2025 The Author(s). Advanced Science published by Wiley-VCH GmbH 21983844, 2025, 34, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.202504746 by Kenji Watanabe - National Institute For , Wiley Online Library on [16/09/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensehttp://www.advancedsciencenews.comhttp://www.advancedscience.comwww.advancedsciencenews.com www.advancedscience.comFigure 1. Artificial vdW ferromagnetic platform for bulk VSe2. a) Schematic illustration of the artificial vdW ferromagnetic platform, which has beenachieved with (i) Ar + H2S plasma and (ii) MFM junction. To spatially resolve the ferromagnetism, an MFM junction has been constructed with amagnetic field generator, magnetic sample holder, and Co-coated magnetic tip, which excludes the generation of the electrical field at the tip-samplejunction. b) AFM image (left side as 3D topography image, right side as error signal image) and c) SEM image of nano-crystallized VSe2.tations in synthetic methodologies, and inherent interfacial inho-mogeneity. Our approach enables artificial vdW ferromagnetismvia nano-crystallization in vdW VSe2. We envision that this strat-egy provides the artificial injection of the vdW ferromagnetism,offering the versatile advances in 2D vdW spintronic systems.2. Results and Discussion2.1. Artificial vdW Ferromagnetic Platform for Bulk VSe2To artificially induce the ferromagnetism of the bulk vdW 1T-VSe2 (non-magnetic), single-step penetrative plasma sulfuriza-tion has been utilized to inject the ferromagnetism in bulk vdWVSe2 via hydrogen sulfide (H2S) + argon (Ar) ion bombardment,which results in the lattice distortion and nano-crystallization.[34]In our previous research, H2S + Ar ion bombardment gen-erates the nano-crystallization in van der Waals materials, of-fering a synthetic platform to isolate the VSe2 monolayer forversatile magnetic functionalities. In this study, this approachhas been extended to distort the vdW lattice in non-magneticbulk VSe2, enabling the emergence of ferromagnetism throughthe VSe2 monolayer isolation. The monolayer VSe2 (1T and 2Hphase) is notable for its intrinsic ferromagnetism owing to thestrong electron coupling in the 3d1 odd-electronic configurationof V4+.[30] Astonishingly, the ferromagnetic ordering of mono-layer VSe2 is robust and persists above room temperature, mak-ing monolayer VSe2 a significant material for vdW spintron-ics applications.[35] However, the monolayer VSe2 is vulnerableto oxidation,[21] which vanishes the ferromagnetism of mono-layer VSe2. Unlike the monolayer VSe2, bulk vdW VSe2 indi-cates non-magnetic properties. Thus, bulk vdW VSe2 was in-tentionally selected for artificial ferromagnetism injection withnano-crystallization. As shown in Figure 1a, the nano-crystallizedVSe2 was fabricated in the following three steps. First, bulk vdWVSe2 was mechanically exfoliated and transferred onto a SiO2/Siwafer. Second, single-step penetrative plasma sulfurization (RFpower 400 W) was conducted to crystallize the bulk vdW VSe2.Third, the MFM junction was constructed for nanoscale observa-tion of the magnetic domain distribution, constructed with a Co-coated magnetic tip (Figure S1, Supporting Information), mag-netic sample holder, and magnetic field generator (Figures S2and S3, Supporting Information), enabling the spatial observa-tion of ferromagnetic characteristics. Also, nano-crystallization ofVSe2 has been observed with AFM and SEM imaging. As shownin Figure 1b, nano-crystallization of VSe2 has been experimen-tally revealed within the AFM3D topography image and error sig-nal image. Furthermore, an SEM image of nano-crystallized VSe2correlatively indicates the nanoscale crystallization. The grainAdv. Sci. 2025, 12, e04746 e04746 (3 of 9) © 2025 The Author(s). Advanced Science published by Wiley-VCH GmbH 21983844, 2025, 34, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.202504746 by Kenji Watanabe - National Institute For , Wiley Online Library on [16/09/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensehttp://www.advancedsciencenews.comhttp://www.advancedscience.comwww.advancedsciencenews.com www.advancedscience.comFigure 2. Cross-sectional observation of nano-crystallized VSe2 via Ar +H2S plasma. a) Schematic illustration of nano-crystallized VSe2, generating theVSe2 ML isolation. b) Cross-sectional analysis of nano-crystallized VSe2 with HR-TEM and STEM image. Cross-sectional d) EDS mapping and e) SAEDpatterns of nano-crystallized VSe2, which is configured with RF plasma 400 W. f) XPS spectra of V 2p, Se 3d, S 2p, exhibiting the sulfurization of bulkvdW VSe2 with emergence of V-S bonding in S 2p spectra.size of nano-crystallized VSe2 is distributed as a function of RFplasma power (18.2–45.7 nm).[36] MFM domain imaging revealsthat the magnetic domain size corresponds with the nanograinsize, resulting in grain boundaries operating as pinning sites. Forthe improvement of large-scale uniformity, inductively coupledplasma (ICP) systems have been utilized to ensure homogeneousion bombardment over centimeter-scale substrates.2.2. Cross-Sectional Observation of Nano-Crystallized VSe2Furthermore, cross-sectional TEM images of nano-crystallizedVSe2 were experimentally obtained, exhibiting the VSe2 mono-layer isolation and its corresponding lattice distortion, as shownin Figure 2a–c. The emergence of room-temperature ferromag-netism in bulk VSe2 is attributed to the VSe2 monolayer isolationvia nano-crystallization. The nano-crystallization process, drivenby local lattice strain during the plasma sulfurization, disruptsinterlayer coherence and effectively decouples adjacent VSe2 lay-ers. This structural decoupling yields electronically quasi-2D re-gions where ferromagnetism prevails, thereby facilitating ferro-magnetic ordering via Stoner-type instability. Concurrently, thelocalized symmetry breaking enhances orbital contributions tomagnetism, further enhancing and stabilizing the ferromagneticbehavior. Collectively, these effects enable the realization of ro-bust ferromagnetism at room temperature in an otherwise non-magnetic bulk VSe2 system. Cross-sectional EDS mapping andSAED pattern were correlated to nano-crystallization. As BulkvdW VSe2 corresponds to Figure S4 (Supporting Information),Figure 2d indicates the nano-crystallized VSe2, comparing the ef-fects of nano-crystallization. While the EDS mapping indicatesthe intrinsic distribution of the V atom, Se atom, C atom, and Satom in bulk states, the distribution of the S atom has been dom-inantly generated at the surface after the nano-crystallization. Asplasma sulfurization is configured with Ar + H2S plasma, re-sulting in the amorphous phase of Bulk vdW VSe2 and nano-crystallization. The SAED pattern of 1T- VSe2 indicates the peri-odic pattern, while the nano-crystallized VSe2 lattice (Figure 2e)experimentally clarifies the origin of the observed unidirectionallattice,[37] which corresponds to the lattice distortion. XPS mea-Adv. Sci. 2025, 12, e04746 e04746 (4 of 9) © 2025 The Author(s). Advanced Science published by Wiley-VCH GmbH 21983844, 2025, 34, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.202504746 by Kenji Watanabe - National Institute For , Wiley Online Library on [16/09/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensehttp://www.advancedsciencenews.comhttp://www.advancedscience.comwww.advancedsciencenews.com www.advancedscience.comsurements were performed to clarify and elucidate variationsof chemical bonding within nano-crystallization, as shown inFigure 2f. As the V 2p XPS spectra of pristine VSe2 have been de-convoluted into the binding energy of 513.3 eV peak, 521.6, and515.4 eV, each peak has been shifted as 517.0, 514.0, 521.9 eVwith nano-crystallization and its corresponding V-S bonding for-mation. Also, S 2p XPS spectra of pristine VSe2 can be separatedas 166.0 eV peak and 160.4 eV peak. After crystallization, an ad-ditional deconvoluted S 2p peak has been generated as 164.5,163.5, and 165.8 eV. Thus, V─S bonding formation and nano-crystallization can be further clarified with a comparison of S2p spectra. Se 3d peak also exhibits heterogeneity in chemicalcomposition, which can be deconvoluted as 54.6, 53.8, and 55 eVpeaks. And Se 3d peak has been shifted to 54.7, 53.9, and 55.3 eV,which directly corresponds to the Se atom termination with sul-furization. Owing to the ion penning effects, Se atoms were lo-cally terminated by S atoms via plasma sulfurization, which re-sulted in a substantial increase in the S/Se atomic concentra-tion ratio. The Se-to-S substitution ratio was quantified fromXPSatomic concentration analysis, yielding sulfur incorporation of≈11.45 at%, while selenium incorporation exhibits ≈7.30 at% atthe nano-crystallized VSe2 (400 W). In our sulfurization system,the sufficient generation of H2S+ for bombardment on VSe2 tocrystallize the lattice is most significant. The proposed mecha-nism of H2S+ generation in this system is the Penning effectby the Ar gas and the direct ionization of H2S as follows Equa-tions (1) and (2).[38]Ar+e− → Ar++2e− (1)Ar+ +H2S → Ar+H2S+ (2)Sufficient electrons in the plasma system can directly ionizeH2S gas to generate H2S+, as shown in Equation (3). But ex-cept for Ar gas, it is difficult to generate H2S plasma owing tothe low ionization energy characteristics of H2S gas.[39] To pre-vent plasma-induced over-etching and maintain the integrity ofthe layered VSe2 structure, plasma conditions were carefully opti-mized. The gas mixture was fixed at a 1:1 ratio of Ar and H2S (50sccm each), and RF plasma power was set at 400 W. These condi-tions were found to be optimal for inducing nano-crystallizationwithout significant damage to the surface or delamination. Pre-liminary experiments with higher RF power (>500 W) or an Ar-rich environment resulted in structural degradation and amor-phization.e− +H2S+ → 2e− (3)For the precise control of plasma-based sulfurization, the gasmixture ratio was fixed as Ar and H2S as 1:1 (50 sccm injectionfor each gas). In the bulk plasma, multi-chain reactions (Equa-tions 1–3) lead to an increase in plasma potential, while the sub-strate remains grounded. This creates a self-biased system thatinduces an electric field (sheath region), accelerating positivelycharged ions (H2S+ and Ar+) toward the substrate and resultingin ion bombardment. This simultaneous ion bombardment onthe single-crystal VSe2 surface induces lattice distortion, break-ing the long-range crystallinity and transforming the surface intoa nanoscale, discontinuous crystalline structure. With continuedion exposure, the bombardment penetrates deeper, affecting sev-eral vdW layers beneath the surface. Consequently, a few up-per layers become nanocrystalline and structurally disordered,while the underlying bulk retains its pristine single-crystallinestructure. This VSe2 monolayer isolation exhibits emergent fer-romagnetic behavior, in contrast to the non-ferromagnetic na-ture of pristine single-crystalline VSe2. The concurrent Ar+ andH2S+ ion bombardment onto single-crystalline VSe2 leads toa high density of nanoscale defects, which disrupts the long-range order and results in nanoscale discontinuous domains ofVSe2. This ion-induced lattice distortion promotes the forma-tion of nanocrystalline structures (Figure S5, Supporting Infor-mation). Similar nano-crystallization phenomena have been ob-served in various systems, including wafer-scale MoS2–WS2 ver-tical heterostructures,[40] WS2–graphene interfaces,[6] and otherTMDC-based heterostructures through plasma-enhanced chem-ical vapor deposition (PECVD).2.3. Spatially-Resolved Ferromagnetic Behavior ofNano-Crystallized VSe2To observe the artificially generated ferromagnetic domain,MFMimage has been correlatively conducted with i) magnetic imag-ing and ii) topography imaging, which allows the observationof long-range magnetic interactions while minimizing the in-fluence of the topography. While the topography imaging wasconducted within a tip-sample distance of ≈5 nm, which affectsthe vdW interaction, magnetic force can be clearly obtained witha tip-sample distance of ≈25 nm. For magnetic field sweep, amagnetic field generator has been attached to control the mag-netic field at the MFM junction. A magnetic field generator wasconstructed with two permanent magnets. With a fixed perma-nent magnet, the rotation of another permanent magnet locallyinduces an in-plane magnetic field at the tip apex between thesoft iron localizers. Rotating the permanent magnet results ina controllable magnetic field between the minimum magneticfield (−500 Oe) and the maximummagnetic field (+500 Oe). Themagnetic field can be controlled at the tip-sample junction, themagnetic hysteresis can be spatially resolved, as shown in Figure3a. As the magnetic field was controlled within 250 Oe duration,the yellow dash box MFM phase images sequentially resolvedas -147.46° (-500 Oe), -148.21° (-250 Oe), -147.43° (0 Oe), 37.95°(+250 Oe), 39.10° (+500 Oe), 38.96° (+500 Oe), 37.01° (+250 Oe),34.88° (0 Oe), -146.90° (-250 Oe), -149.0° (-500 Oe). In contrast,the white dashed box in the MFM phase image can be mappedas 38.90° (-500 Oe), -39.28° (-250 Oe), -37.16° (0 Oe), -144.63°(+250 Oe), -146.72° (+500 Oe), -145.18° (+500 Oe), -145.94°(+250Oe), -145.16° (0 Oe), 38.55° (-250Oe), 39.04° (-500Oe). Fur-thermore, the ferromagnetic hysteresis curve has been mappedfrom spatially extracted ferromagnetic phase value from eachdashed box, as shown in Figure 3b. Owing to the MFM phasemapping, the nanoscale ferromagnetic domain has been exper-imentally observed with room-temperature ferromagnetic hys-teresis behavior. Regarding the emergence of room-temperatureferromagnetism in bulk VSe2 upon Ar +H2S plasma treatment,the synergistic mechanism has been attributed to i) orbital mag-netism and ii) vdW sulfur intercalation, which effectively iso-lates monolayer VSe2 regions at the bulk VSe2 crystal. First, theAdv. Sci. 2025, 12, e04746 e04746 (5 of 9) © 2025 The Author(s). Advanced Science published by Wiley-VCH GmbH 21983844, 2025, 34, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.202504746 by Kenji Watanabe - National Institute For , Wiley Online Library on [16/09/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensehttp://www.advancedsciencenews.comhttp://www.advancedscience.comwww.advancedsciencenews.com www.advancedscience.comFigure 3. Spatially-resolved ferromagnetism of nano-crystallized VSe2. Resolving the nanoscale magnetic heterogeneity and ferromagnetic hysteresisbehavior via magnetic domain imaging. a) sequential MFM phase images of nano-crystallized VSe2, which has been generated by the magnetic fieldcontrol. b) Ferromagnetic hysteresis mapping with nanoscale magnetic domain extraction from the selected yellow box (left) and white box (right).nano-crystallization process introduces substantial local strainand atomic disorder into the VSe2 lattice. These structural per-turbations break the spatial inversion symmetry and promote thelocalization of vanadium 3d orbitals, thereby enhancing orbitalmagnetic moments. Such orbital contributions are known to playa critical role in transition metal dichalcogenide systems underreduced symmetry, enabling finite magnetization even in the ab-sence of conventional spin ordering. Density functional theory(DFT) calculations on disordered VSe2 supercells further supportthis scenario, indicating non-zero net magnetic moments arisingfrom asymmetric d-orbital occupancy.[41] Second, the incorpora-tion of sulfur atoms during H2S plasma exposure induces theintercalation of sulfur species into the vdW gaps between VSe2layers. This interlayer sulfur intercalation disrupts the electroniccoherence along the c-axis, effectively decoupling adjacent VSe2layers and inducing quasi-monolayer behavior within localizedcrystalline domains. Previous theoretical and experimental stud-ies have established that monolayer VSe2 favors itinerant ferro-magnetism due to Stoner-type instability at the Fermi level,[42]a behavior suppressed in the bulk form due to strong interlayerhybridization. Our results suggest that the plasma-induced sul-fur intercalation restores the monolayer-like electronic structurewithin nano-crystallized grains, enabling ferromagnetic orderingat room temperature. Thus, the emergence of room-temperatureferromagnetism in sulfurized VSe2 arises from a cooperative in-terplay between orbital magnetism driven by lattice disorder andmonolayer isolation effects. This post-synthetic mechanism rep-resents a novel pathway to modulate the ferromagnetic order inotherwise non-magnetic vdW materials.2.4. Nano-Crystallization Effects in the Artificially GeneratedFerromagnetic DomainWithin the magnetic field weep, MFM phase (Figure 4a) andMFM amplitude (Figure 4b) from opposite magnetic fieldsAdv. Sci. 2025, 12, e04746 e04746 (6 of 9) © 2025 The Author(s). Advanced Science published by Wiley-VCH GmbH 21983844, 2025, 34, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.202504746 by Kenji Watanabe - National Institute For , Wiley Online Library on [16/09/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensehttp://www.advancedsciencenews.comhttp://www.advancedscience.comwww.advancedsciencenews.com www.advancedscience.comFigure 4. Reversible magnetization of nano-crystalline ferromagnetic domain. a)MFMphase images (top) and b)MFM amplitude images (bottom) witha heterogeneous magnetic field. Pixel distribution of nano-crystallized VSe2, consisted of c) MFM phase and d) MFM amplitude. e) Cross-sectional lineprofiles of MFM amplitude, which indicates magnetization reversal of nano-crystallized VSe2. f) Sequential domain dynamics with magnetic field sweep,resulting in the magnetization reversal of the ferromagnetic domain. g) ferromagnetic hysteresis with RF plasma power variation and its correspondingh) coercivity.(+500 Oe, -500 Oe) correspond to the magnetization reversal,which fully operates as a reversible magnet. Furthermore, statis-tical analysis with nano-crystallized VSe2 MFM pixel distributionhas been conducted, as shown in Figure 4c,d.As shown in Figure 4c, the dominant pixel peak from +500 Oecorresponds to the MFM phase as -101.89°, while the dominantpixel peak with−500 Oe has been extracted as 1.36°. Additionally,MFM amplitude pixel mapping exhibits heterogeneous peak dis-tribution of 505.67° and 476.45°, correlating the existence of theheterogeneous magnetic pole (Figure 4d). Such reversible pixeldistribution from MFM phase and MFM amplitude images di-rectly supports the magnetization reversal. The cross-sectionalline profile of nano-crystallized VSe2 corresponds to the mag-netization reversal within magnetic field control (Figure 4e). Toverify that the nano-crystallization effects for ferromagnetism,magnetization reversal (Figure S6, Supporting Information), anddomain pinning effects were also resolved with MFM ampli-tude images (Figure 4f). Within the maximum magnetic field(+500 Oe, -500 Oe), domain distribution of +250 Oe, -250 Oehas been expanded owing to the atomic-scale defects from nano-crystallization, which induces the domain pinning effects. Theemergence of the nanoscale ferromagnetic domain can be ex-Adv. Sci. 2025, 12, e04746 e04746 (7 of 9) © 2025 The Author(s). Advanced Science published by Wiley-VCH GmbH 21983844, 2025, 34, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.202504746 by Kenji Watanabe - National Institute For , Wiley Online Library on [16/09/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensehttp://www.advancedsciencenews.comhttp://www.advancedscience.comwww.advancedsciencenews.com www.advancedscience.complained with nano-crystallization. When pinning effects are neg-ligible, magnetic domain walls can be spatially shifted and ex-panded without significant domain wall resistance, leading tohigh initial magnetization within a minimum external magneticfield. However, the existence of defects enhances the energy bar-rier of ferromagnetic domain wall movements, which completelyblocks the spatial domain wall movements. Regarding the highdefect density of nano-crystallized VSe2, the magnetization risesgradually until the external magnetic field is as large as thepinning energy. To further validate the room-temperature fer-romagnetism of nano-crystallized VSe2, bulk VSe2 has been in-vestigated with MFM imaging and its corresponding pixel dis-tribution mapping (Figures S7–S10, Supporting Information).As bulk VSe2 exhibits non-magnetic properties, magnetizationreversal, ferromagnetic hysteresis, and domain pinning effectswere not experimentally observed, unlike nano-crystallized VSe2.To verify the room-temperature ferromagnetism observed viaMFM, superconducting quantum interference device (SQUID)magnetometry was performed on nano-crystallized VSe2. Asshown in Figure 4g, the M–H loop at 300 K demonstrates theenlargement of ferromagnetic hysteresis and its correspond-ing coercivity as ≈0.009 mT (300 W), 0.057 mT (350 W), and0.083mT (400W). Plasma-dependent coercivity further indicatesa nano-crystallization of bulk VSe2, substantiating the room-temperature ferromagnetic behavior in our system.3. ConclusionIn conclusion, an artificial room-temperature vdW ferromag-netism has been achieved in VSe2 through nano-crystallizationwith plasma sulfurization. Owing to the ion bombardment, theSe atom is randomly terminated to the S atom, resulting in theVSe2 monolayer isolation and local lattice distortion. By con-structing the MFM junction with nano-crystallized VSe2, vdWferromagnetism, and its corresponding ferromagnetic hysteresiscurve have been spatially resolved. Nano-crystallization of bulkvdW VSe2 was also correlatively observed with cross-sectionaltransmission electron microscopy, energy-dispersive X-ray spec-troscopy, and selected area diffraction analysis. In conclusion,our artificial room-temperature vdW ferromagnetic platform canoffer an extendable platform for vdW ferromagnetic material,which enables the vdW ferromagnets to be accessible, engineer-able, and integrable into emergent heterostructures for previ-ously unachieved.4. Experimental SectionNano-Crystallization: The ICP-type of plasma-enhanced chemical va-por deposition (ICP-PECVD) (AFS-IC6T, Korea) was used for the crystal-lization of VSe2 to induce its amorphous phase. A high vacuum of ≈5 ×10−5 in the PECVD chamber was used to evacuate impurities to achieveclean synthesis without other unexpected reactions before plasma treat-ment for nano-crystallization. In this study, only the RF plasma power wasfixed as 400 W under constant gas conditions, and the argon and H2Sflows were maintained at 50 SCCM at a pressure of 25 mTorr at room tem-perature.Mechanical Exfoliation and Transfer of vdW VSe2: Before mechanicalexfoliation and dry transfer, a polydimethylsiloxane stamp was attachedto a glass cover. vdW VSe2 was mechanically exfoliated from bulk crystals(HQGraphene, Netherlands) onto polydimethylsiloxane stamps and thentransferred onto the substrate by applying a transfer condition of 70 °C.Magnetic Force Microscopy: MFM (NX-10 AFM, Park Systems, Repub-lic of Korea) was conducted with an MFMR cantilever. The MFMR can-tilever was calibrated with a tip radius of 25 nm, a length of 225 μm, aheight of 15 μm, a width of 28 μm, and a spring constant of 2.8 N/m,resulting in a resonance frequency of 75 kHz. A magnetic sample holderwas loaded to block the electrical field generation at the MFM junction.Additionally, a magnetic field generator was further attached to artificiallyinduce the magnetic field and observe the magnetic hysteresis, which wasspatially resolved at the MFM junction. Before the MFM measurements,the MFM tip was magnetized as an “N” pole for 15 min.Material Characterization: XPS measurements (XIS Supra+, Kratos,United Kingdom) were used to characterize VSe2, with an X-ray spot sizeof 400 μm. Peak deconvolution was performed on the V 2p, Se 2p, and S2p signals, with the profiles aligned using the C 1s peak at 285 eV. The XPSdata were calibrated using the CASAXPS software (version 8.1). Opticalmicroscopy (U-MSSP4, Olympus, Japan) and FE-SEM (S-4800, Hitachi,Japan) were used to examine the transferred flakes. For cross-sectionalTEM specimen preparation, a focused ion beam instrument (NX2000, Hi-tachi Ltd., Japan) was used, employing a Ga+ ion beam (30–5 keV) anda lift-off process to etch the specimens. TEM (JEM-2100F, JEOL, Japan)and XRD (Empyrean, Malvern PANalytical, United Kingdom) were used toobserve the lattice structure, EDS, and SAED patterns of the layered VSe2structures at the atomic scale.Supporting InformationSupporting Information is available from the Wiley Online Library or fromthe author.AcknowledgementsThis research was supported by the Basic Science Research Program of theNational Research Foundation of Korea (NRF) funded by the Ministry ofEducation (No. 2022R1A3B1078163). This study was supported by the In-stitute for Basic Science (grant number IBS-R027-D1). This work was sup-ported by the Korean Collaborative & High-tech Initiative for ProspectiveSemiconductor Research (K-CHIPS) (20024772), funded by the Ministryof Trade, Industry & Energy (MOTIE, Korea). This study was supportedby the MOTIE (Ministry of Trade, Industry, and Energy (grant number1415187508) for the development of future semiconductor devices. Thisstudy was supported by the National Research Foundation (NRF) fundedby the Korean government (MSIT) (No. RS-2024-00437142). This workwas supported by the Technology Innovation Program (20017367, Devel-opment of precise manufacturing technology for CMP pad conditioners),funded By the Ministry of Trade, Industry & Energy (MOTIE, Korea).Conflict of InterestThe authors declare no conflict of interest.Author ContributionsJ.L., G.K., H.S., H.C. contributed equally to this work. J.L., G.K., H.S., andH.C. prepared samples and performed experiments. H.L., S.L., G.K., H.K.,S.S., S.S., and D.L. performed the technical discussions on plasma sulfu-rization. H.S., S.H., G.B., H.H. conducted the analytical experiments, in-cluding TEM, EDS, and XPS measurements. G.H., G.J., and Y.L. providedtechnical advice on the MFM system and magnetic field generator. T.T.and K.W. provide the bulk hexagonal boron nitride samples. A.O., Y.K.,and L.F. A.H., W.J., W. S., S.C., H.K., J.L., G.K., H.S., H.C. and T.K. wrotethe manuscript with contributions from all the authors. T.K. designed andsupervised the study. All the authors have read and approved the final ver-sion of this manuscript.Adv. Sci. 2025, 12, e04746 e04746 (8 of 9) © 2025 The Author(s). Advanced Science published by Wiley-VCH GmbH 21983844, 2025, 34, Downloaded from https://advanced.onlinelibrary.wiley.com/doi/10.1002/advs.202504746 by Kenji Watanabe - National Institute For , Wiley Online Library on [16/09/2025]. 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See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensehttp://www.advancedsciencenews.comhttp://www.advancedscience.com Artificial Room-Temperature Ferromagnetism of Bulk van der Waals VSe2 1. Introduction 2. Results and Discussion 2.1. Artificial vdW Ferromagnetic Platform for Bulk VSe2 2.2. Cross-Sectional Observation of Nano-Crystallized VSe2 2.3. Spatially-Resolved Ferromagnetic Behavior of Nano-Crystallized VSe2 2.4. Nano-Crystallization Effects in the Artificially Generated Ferromagnetic Domain 3. Conclusion 4. Experimental Section Supporting Information Acknowledgements Conflict of Interest Author Contributions Data Availability Statement Keywords