Complex Magnetic Behavior in RuO2 Thin Films Driven by Strain and Substrate Effects

Complex Magnetic Behavior in RuO2 Thin Films Driven by Strain and Substrate Effects | 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 Complex Magnetic Behavior in RuO2 Thin Films Driven by Strain and Substrate Effects Mojtaba Alaei, Nafise Rezaei, Ilia Mikhailov, Artem R. Oganov, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8958016/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 Ruthenium dioxide (RuO$_2$) has been proposed as a prototypical metallic $d$-wave altermagnet, a Néel-ordered compensated antiferromagnetic state exhibiting nonrelativistic momentum-dependent spin splitting; yet, its magnetic ground state remains controversial both theoretically and experimentally. Using comprehensive first-principles calculations, we investigate RuO$_2$ thin films with (110), (100), and (001) orientations, both (un)strained freestanding and supported on a TiO$_2$ substrate. We show that emergent magnetic moments in RuO$_2$ thin films are highly fragile, strongly influenced by strain, surface orientation, and atomic relaxation, while also being highly sensitive to the choice of the Brillouin-zone integration scheme. We find that none of the thin film structures considered can stabilize a compensated antiferromagnetic order; therefore, an altermagnetic ground state cannot be realized. Instead, substrate-supported RuO$_2$ films on TiO$_2$ exhibit pronounced layer- and site-dependent magnetic moment variations and incomplete compensation between the two antiferromagnetically coupled Ru moments, yielding a \emph{ferrimagnetic-like} behavior. On the other hand, freestanding RuO$_2$ films display complex magnetic structures depending on their orientation and applied strain, with distinct behavior at the surfaces and in the inner layers. Our results reconcile conflicting theoretical and experimental reports and underscore the sensitivity of RuO$_2$ magnetism to structural and methodological details. Physical sciences/Materials science/Condensed-matter physics/Magnetic properties and materials Physical sciences/Materials science/Theory and computation/Electronic structure Physical sciences/Materials science/Nanoscale materials/Two-dimensional materials Full Text Additional Declarations There is NO Competing Interest. 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. 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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-8958016","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":615880174,"identity":"f001bfed-e40d-42ee-beb5-7d70ac1c05ec","order_by":0,"name":"Mojtaba Alaei","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA0klEQVRIie3OsQqCUBSA4ROCLddaLxT5BMGNIJp8FsXBpUJocZBwskXwEXoFe4MjF2y5voPtDY4tSdrYoLet4f7T4XA+OAAq1X82QgC6APIZwJYyHVm3BBB/IOBE0mQZaRU+g613STjyOrAOMBOsl2xQZ3ki6D4rYxtRuEeY7IYIMDTilkwJwzzG9kMyRMZ1/mqoZ6YdaaQIYdyIqA1l0pJIhnDi83lBV5kobBSF68RE9/vJ7Xy9P8KTaSZuXgWh5aREy3oJaN8Lvf9epVKpVDK9Af4QTUSy26AhAAAAAElFTkSuQmCC","orcid":"https://orcid.org/0000-0002-8023-9761","institution":"Isfahan University of Technology","correspondingAuthor":true,"prefix":"","firstName":"Mojtaba","middleName":"","lastName":"Alaei","suffix":""},{"id":615880175,"identity":"06188cbe-d4b8-4e31-941b-61991ccff73d","order_by":1,"name":"Nafise Rezaei","email":"","orcid":"https://orcid.org/0009-0000-0185-2449","institution":"","correspondingAuthor":false,"prefix":"","firstName":"Nafise","middleName":"","lastName":"Rezaei","suffix":""},{"id":615880176,"identity":"d49a2cbc-c725-47e6-8b82-079faff973b6","order_by":2,"name":"Ilia Mikhailov","email":"","orcid":"","institution":"","correspondingAuthor":false,"prefix":"","firstName":"Ilia","middleName":"","lastName":"Mikhailov","suffix":""},{"id":615880177,"identity":"2b4809bf-4d93-49fc-8933-edcf671b7c4a","order_by":3,"name":"Artem R. 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Using comprehensive first-principles calculations, we investigate RuO$_2$ thin films with (110), (100), and (001) orientations, both (un)strained freestanding and supported on a TiO$_2$ substrate. We show that emergent magnetic moments in RuO$_2$ thin films are highly fragile, strongly influenced by strain, surface orientation, and atomic relaxation, while also being highly sensitive to the choice of the Brillouin-zone integration scheme. We find that none of the thin film structures considered can stabilize a compensated antiferromagnetic order; therefore, an altermagnetic ground state cannot be realized. Instead, substrate-supported RuO$_2$ films on TiO$_2$ exhibit pronounced layer- and site-dependent magnetic moment variations and incomplete compensation between the two antiferromagnetically coupled Ru moments, yielding a \\emph{ferrimagnetic-like} behavior. On the other hand, freestanding RuO$_2$ films display complex magnetic structures depending on their orientation and applied strain, with distinct behavior at the surfaces and in the inner layers. Our results reconcile conflicting theoretical and experimental reports and underscore the sensitivity of RuO$_2$ magnetism to structural and methodological details.","manuscriptTitle":"Complex Magnetic Behavior in RuO2 Thin Films Driven by Strain and Substrate\nEffects","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-04-20 15:04:44","doi":"10.21203/rs.3.rs-8958016/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"communications-materials","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"commsmat","sideBox":"Learn more about [Communications Materials](https://www.nature.com/commsmat/)","snPcode":"","submissionUrl":"","title":"Communications Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Communications Series","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"30af33d4-4025-4d3e-9c56-e0d47bd728a7","owner":[],"postedDate":"April 20th, 2026","published":true,"recentEditorialEvents":[{"type":"reviewerAgreed","content":"This content is not available.","date":"2026-05-04T04:44:56+00:00","index":5,"fulltext":"This content is not available."},{"type":"reviewerAgreed","content":"This content is not available.","date":"2026-04-29T08:22:08+00:00","index":4,"fulltext":"This content is not available."}],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":65538321,"name":"Physical sciences/Materials science/Condensed-matter physics/Magnetic properties and materials"},{"id":65538322,"name":"Physical sciences/Materials science/Theory and computation/Electronic structure"},{"id":65538323,"name":"Physical sciences/Materials science/Nanoscale materials/Two-dimensional materials"}],"tags":[],"updatedAt":"2026-04-20T15:04:44+00:00","versionOfRecord":[],"versionCreatedAt":"2026-04-20 15:04:44","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-8958016","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8958016","identity":"rs-8958016","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}