Experimental Observation of Altermagnetism in Twisted CrPS₄ van der Waals Homostructures

Experimental Observation of Altermagnetism in Twisted CrPS₄ van der Waals Homostructures | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Experimental Observation of Altermagnetism in Twisted CrPS₄ van der Waals Homostructures Yanping Liu, Junying Chen, Xing Xie, Shaofei Li, Siyu Zhang, Shikun Hou, and 4 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7958512/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted You are reading this latest preprint version Abstract Altermagnetism, characterized by compensated antiparallel spin order with finite spin splitting, bridges the properties of ferromagnets and antiferromagnets and holds great promise for next-generation spintronic applications. Theoretical studies suggest that twisting van der Waals (vdW) layers can generate altermagnetic states by engineering the interlayer symmetry, thereby expanding the family of magnetic quantum materials. However, direct experimental observation of altermagnetism in these vdW systems remains elusive. Here, we present experimental evidence to demonstrate the realization of altermagnetism in orthogonally twisted CrPS4/CrPS4 (90°- CrPS4/CrPS4) homostructures using magneto-optical spectroscopy. The symmetry of 90°-CrPS4/CrPS4 exhibits a ferromagnetic-like magnetic-field-dependent degree of circular polarization (DOCP), showing opposite variations under σ⁺ and σ⁻ excitations as the field sweeps from –9 T to 9 T. Moreover, a pronounced Zeeman splitting of ~2 meV—absent in either ferromagnetic or antiferromagnetic CrPS4—emerges in the twisted configuration, indicating a unique magnetic ground state. First-principles calculations reveal large spin-split bands in an antiferromagnetic configuration, confirming the realization of altermagnetism in 90°- CrPS4/ CrPS4. Polarized Raman spectroscopy further identifies interlayer-coupling-induced phonon mode splitting unique to the altermagnetic state. These findings provide the first experimental observation of altermagnetism in a twisted vdW material and establish a versatile platform for engineering symmetry-driven spin-split states, opening new avenues for spintronic and quantum information technologies. Physical sciences/Materials science/Condensed-matter physics/Magnetic properties and materials Physical sciences/Materials science/Nanoscale materials/Magnetic properties and materials Altermagnetism orthogonally twisted CrPS4/CrPS4 Zeeman splitting Raman splitting magneto-optical spectroscopy Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupportingInformation.pdf Supporting Information Cite Share Download PDF Status: Under Review Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-7958512","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":616421949,"identity":"341a510b-eb3f-4066-b6fd-21bb768002bf","order_by":0,"name":"Yanping 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spectroscopy","lastPublishedDoi":"10.21203/rs.3.rs-7958512/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7958512/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Altermagnetism, characterized by compensated antiparallel spin order with finite spin splitting, bridges the properties of ferromagnets and antiferromagnets and holds great promise for next-generation spintronic applications. Theoretical studies suggest that twisting van der Waals (vdW) layers can generate altermagnetic states by engineering the interlayer symmetry, thereby expanding the family of magnetic quantum materials. However, direct experimental observation of altermagnetism in these vdW systems remains elusive. Here, we present experimental evidence to demonstrate the realization of altermagnetism in orthogonally twisted CrPS4/CrPS4 (90°- CrPS4/CrPS4) homostructures using magneto-optical spectroscopy. The symmetry of 90°-CrPS4/CrPS4 exhibits a ferromagnetic-like magnetic-field-dependent degree of circular polarization (DOCP), showing opposite variations under σ⁺ and σ⁻ excitations as the field sweeps from –9 T to 9 T. Moreover, a pronounced Zeeman splitting of ~2 meV—absent in either ferromagnetic or antiferromagnetic CrPS4—emerges in the twisted configuration, indicating a unique magnetic ground state. First-principles calculations reveal large spin-split bands in an antiferromagnetic configuration, confirming the realization of altermagnetism in 90°- CrPS4/ CrPS4. Polarized Raman spectroscopy further identifies interlayer-coupling-induced phonon mode splitting unique to the altermagnetic state. These findings provide the first experimental observation of altermagnetism in a twisted vdW material and establish a versatile platform for engineering symmetry-driven spin-split states, opening new avenues for spintronic and quantum information technologies.","manuscriptTitle":"Experimental Observation of Altermagnetism in Twisted CrPS₄ van der Waals Homostructures","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-04-03 04:54:27","doi":"10.21203/rs.3.rs-7958512/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-physics","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"nphys","sideBox":"Learn more about [Nature Physics](http://www.nature.com/nphys/)","snPcode":"","submissionUrl":"","title":"Nature Physics","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Research","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"ce84e186-ebe8-4397-b6c8-b46949daac6b","owner":[],"postedDate":"April 3rd, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":65595305,"name":"Physical sciences/Materials science/Condensed-matter physics/Magnetic properties and materials"},{"id":65595306,"name":"Physical sciences/Materials science/Nanoscale materials/Magnetic properties and materials"}],"tags":[],"updatedAt":"2026-04-03T04:54:27+00:00","versionOfRecord":[],"versionCreatedAt":"2026-04-03 04:54:27","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-7958512","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7958512","identity":"rs-7958512","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}