Noncollinear ferrielectricity in a van der Waals crystal

Noncollinear ferrielectricity in a van der Waals crystal | 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 Noncollinear ferrielectricity in a van der Waals crystal Cheng-Yan Xu, Jierui Fu, Gang Wang, Wen He, Yuqiang Fang, Yanting Peng, and 23 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6930601/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 19 Mar, 2026 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Inspired by noncollinear magnetic dipole order, the noncollinear electric dipole order is anticipated to induce rich ferroelectric physics for fascinating device applications. However, establishing noncollinear electric dipole ordering in single crystals is challenging due to electric polarization locking to the crystallographic axes. Here, we report the noncollinear ferrielectricity in a van der Waals crystal WO2Br2 by introducing the competition of ferroelectric and antiferroelectric modes, and uncover its critical role on the polarization switching under hydrostatic pressure and coherent phonon dynamics. The noncollinear dipole order of WO2Br2 was revealed by decoupling the antipolar displacement component along the b-axis and the polar component along the c-axis, both of which were directly visualized by scanning transmission electron microscopy (STEM). Moreover, this noncollinear dipole order not only drives the robust in-plane uniaxial macroscopic ferroelectric behavior, but also enables 90° polarization flip under hydrostatic pressure with two energetically degenerate transition pathways: one via an antipolar intermediate phase, the other through a 45° polar phase respectively. Specially, ultrafast electron diffraction measurements confirm that optical excitation drives two distinct coherent phonon modes associated with the ferroelectric and antiferroelectric orders respectively, shedding light on ultrafast control of the exotic noncollinear ferroelectric states. Our work definitely unlocks the underlying physics of noncollinear ferroelectricity for emergent ferroelectric device applications. Physical sciences/Materials science/Nanoscale materials/Two-dimensional materials Physical sciences/Materials science/Condensed-matter physics/Ferroelectrics and multiferroics Full Text Additional Declarations There is NO Competing Interest. Supplementary Files 20251217supplementaryinformation.pdf Supplementary information Cite Share Download PDF Status: Published Journal Publication published 19 Mar, 2026 Read the published version in Nature Communications → 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-6930601","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":573121733,"identity":"177f620b-4478-45c5-8137-988fbe9d05ea","order_by":0,"name":"Cheng-Yan Xu","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAtklEQVRIiWNgGAWjYNCCigM8IEqCBC1nDvDwkKaFse0AA/Fa+GcksEnzzrsjY8/AfPA2D4NdHkEtEjcSmI15tz0DOowt2ZqHIbmYoBYDiQTGx7zbDgO18JhJ8zAcSGwgQgvDYd45IC3834jWArSlAWwLG3FaJM48YDaccwyo5TCbseUcg2TCWvjbE9gk3tQctmdvb354402FHWEtDAL5HyAMZrA7CaoHWXOAGFWjYBSMglEwogEA7aQxJrjEAiMAAAAASUVORK5CYII=","orcid":"https://orcid.org/0000-0002-7835-6635","institution":"Sauvage Laboratory for Smart Materials, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen)","correspondingAuthor":true,"prefix":"","firstName":"Cheng-Yan","middleName":"","lastName":"Xu","suffix":""},{"id":573121734,"identity":"94d268ab-d16f-4824-9e20-c2d81fbd0195","order_by":1,"name":"Jierui Fu","email":"","orcid":"","institution":"School of Materials Science and Engineering, Harbin Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Jierui","middleName":"","lastName":"Fu","suffix":""},{"id":573121735,"identity":"78447693-8e59-4731-89a3-208824de6033","order_by":2,"name":"Gang Wang","email":"","orcid":"https://orcid.org/0009-0001-3052-2745","institution":"Southern University of Science and Technology","correspondingAuthor":false,"prefix":"","firstName":"Gang","middleName":"","lastName":"Wang","suffix":""},{"id":573121736,"identity":"20cfa104-0dee-480a-afdb-72047e293b0e","order_by":3,"name":"Wen He","email":"","orcid":"https://orcid.org/0000-0001-7972-8667","institution":"School of Materials Science and Engineering, Harbin Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Wen","middleName":"","lastName":"He","suffix":""},{"id":573121737,"identity":"9a9da0fe-390c-4a6b-995f-eb1918fb068e","order_by":4,"name":"Yuqiang Fang","email":"","orcid":"","institution":"Shanghai Jiaotong University","correspondingAuthor":false,"prefix":"","firstName":"Yuqiang","middleName":"","lastName":"Fang","suffix":""},{"id":573121738,"identity":"43c8c9ee-cf3c-432f-9381-f5a74575df84","order_by":5,"name":"Yanting Peng","email":"","orcid":"","institution":"School of Aerospace Engineering, Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Yanting","middleName":"","lastName":"Peng","suffix":""},{"id":573121739,"identity":"4ba2dbb2-0df8-4f8f-a609-7724675b6544","order_by":6,"name":"Dong Wang","email":"","orcid":"https://orcid.org/0000-0001-5004-9732","institution":"Center for High Pressure Science and Technology Advanced Research (HPSTAR)","correspondingAuthor":false,"prefix":"","firstName":"Dong","middleName":"","lastName":"Wang","suffix":""},{"id":573121740,"identity":"3ce3b4b0-3755-4715-81d5-78bf12e88eb7","order_by":7,"name":"Zhenjie Guan","email":"","orcid":"","institution":"School of Materials Science and Engineering, Harbin Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Zhenjie","middleName":"","lastName":"Guan","suffix":""},{"id":573121741,"identity":"538f764f-52bf-4eef-ba8d-893e469623ec","order_by":8,"name":"Xuzhou Sun","email":"","orcid":"","institution":"School of Materials Science and Engineering, Shanghai Jiao Tong University","correspondingAuthor":false,"prefix":"","firstName":"Xuzhou","middleName":"","lastName":"Sun","suffix":""},{"id":573121742,"identity":"946f5448-4c98-4563-a070-8ee7762e53a9","order_by":9,"name":"Shuming Zhang","email":"","orcid":"","institution":"School of Physics, Zhejiang University","correspondingAuthor":false,"prefix":"","firstName":"Shuming","middleName":"","lastName":"Zhang","suffix":""},{"id":573121743,"identity":"79d64951-dc6c-41a0-b915-72bf90063294","order_by":10,"name":"Zunyi Deng","email":"","orcid":"https://orcid.org/0000-0002-4127-7407","institution":"Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Zunyi","middleName":"","lastName":"Deng","suffix":""},{"id":573121744,"identity":"87fa28c1-2d1a-4aa5-a385-89c544b95340","order_by":11,"name":"Gang Tang","email":"","orcid":"","institution":"Zhuhai Beijing Institute of Technology (BIT)","correspondingAuthor":false,"prefix":"","firstName":"Gang","middleName":"","lastName":"Tang","suffix":""},{"id":573121745,"identity":"0850172e-9a0c-404d-a68b-49566e3a89b4","order_by":12,"name":"Yue Liu","email":"","orcid":"","institution":"School of Materials Science and Engineering, Harbin Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Yue","middleName":"","lastName":"Liu","suffix":""},{"id":573121746,"identity":"3c9b1f26-5004-4c30-86aa-24517d11b8c9","order_by":13,"name":"Jiapeng Wang","email":"","orcid":"","institution":"School of Materials Science and Engineering, Harbin Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Jiapeng","middleName":"","lastName":"Wang","suffix":""},{"id":573121747,"identity":"2333e8b3-b7e5-46de-92d7-366839c1af62","order_by":14,"name":"Songge Li","email":"","orcid":"","institution":"Southern University of Science and Technology","correspondingAuthor":false,"prefix":"","firstName":"Songge","middleName":"","lastName":"Li","suffix":""},{"id":573121748,"identity":"6464b319-a0b3-4399-b6af-eef9b7f4ebea","order_by":15,"name":"Tingting Li","email":"","orcid":"","institution":"Department of Physics and Shenzhen Key Laboratory of Advanced Quantum Functional Materials and Devices, Southern University of Science and Technology","correspondingAuthor":false,"prefix":"","firstName":"Tingting","middleName":"","lastName":"Li","suffix":""},{"id":573121749,"identity":"0adceb5f-e29f-421c-91b9-a70cf664a368","order_by":16,"name":"Jinjing Zhou","email":"","orcid":"","institution":"School of Materials Science and Engineering, Harbin Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Jinjing","middleName":"","lastName":"Zhou","suffix":""},{"id":573121750,"identity":"d72ebeb3-6139-4592-9312-57d8c5e30e37","order_by":17,"name":"Yuchen Shang","email":"","orcid":"","institution":"Jilin University","correspondingAuthor":false,"prefix":"","firstName":"Yuchen","middleName":"","lastName":"Shang","suffix":""},{"id":573121751,"identity":"f853b565-3384-4d45-9e37-57b6889265b7","order_by":18,"name":"Yankun Yin","email":"","orcid":"https://orcid.org/0009-0006-7775-1517","institution":"Jilin University","correspondingAuthor":false,"prefix":"","firstName":"Yankun","middleName":"","lastName":"Yin","suffix":""},{"id":573121752,"identity":"77522700-d753-446f-853a-f26e4cdde84f","order_by":19,"name":"Zhaoju Yang","email":"","orcid":"https://orcid.org/0000-0002-9880-2655","institution":"Zhejiang University","correspondingAuthor":false,"prefix":"","firstName":"Zhaoju","middleName":"","lastName":"Yang","suffix":""},{"id":573121753,"identity":"4f5b7d16-d7bc-42b0-9bca-eb75ec4006d9","order_by":20,"name":"Jinzhong Wang","email":"","orcid":"","institution":"School of Materials Science and Engineering, Harbin Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Jinzhong","middleName":"","lastName":"Wang","suffix":""},{"id":573121754,"identity":"7976f7a1-0831-484f-be09-ffe278fd25d2","order_by":21,"name":"Yang Ding","email":"","orcid":"https://orcid.org/0000-0002-6807-3295","institution":"Center for High Pressure Science and Technology Advanced Research","correspondingAuthor":false,"prefix":"","firstName":"Yang","middleName":"","lastName":"Ding","suffix":""},{"id":573121755,"identity":"a70e23eb-5743-40af-b345-0c2fd0946c24","order_by":22,"name":"Liang Zhen","email":"","orcid":"https://orcid.org/0000-0001-6159-8972","institution":"School of Materials Science and Engineering, Harbin Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Liang","middleName":"","lastName":"Zhen","suffix":""},{"id":573121756,"identity":"1dca465f-d5eb-4225-a2a2-644febb4cc5d","order_by":23,"name":"Jiawang Hong","email":"","orcid":"https://orcid.org/0000-0002-9915-8072","institution":"School of Aerospace Engineering \u0026 State Key Laboratory of Environment Characteristics and Effects for Near-space, Beijing Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Jiawang","middleName":"","lastName":"Hong","suffix":""},{"id":573121757,"identity":"eebfe0a9-bba0-450a-ac8e-8ea74603ceef","order_by":24,"name":"Fuqiang Huang","email":"","orcid":"https://orcid.org/0000-0003-0526-5473","institution":"School of Materials Science and Engineering, Shanghai Jiao Tong University","correspondingAuthor":false,"prefix":"","firstName":"Fuqiang","middleName":"","lastName":"Huang","suffix":""},{"id":573121758,"identity":"1b11f525-2da5-4e3f-a639-481c82e65df7","order_by":25,"name":"Junhao Lin","email":"","orcid":"https://orcid.org/0000-0002-2195-2823","institution":"Southern University of Science and Technology","correspondingAuthor":false,"prefix":"","firstName":"Junhao","middleName":"","lastName":"Lin","suffix":""},{"id":573121759,"identity":"7548ba5c-1202-4fc8-bfe3-2f029ca7555e","order_by":26,"name":"Yang Li","email":"","orcid":"https://orcid.org/0009-0005-9836-2556","institution":"School of Materials Science and Engineering, Harbin Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Yang","middleName":"","lastName":"Li","suffix":""},{"id":573121760,"identity":"2e83ef50-4883-4dc3-a5f0-1475b24f5070","order_by":27,"name":"Yingpeng Qi","email":"","orcid":"https://orcid.org/0000-0001-5950-8157","institution":"Shanghai Jiao Tong University","correspondingAuthor":false,"prefix":"","firstName":"Yingpeng","middleName":"","lastName":"Qi","suffix":""},{"id":573121761,"identity":"97aeebd8-f5c3-4808-9f29-4a371c1764c5","order_by":28,"name":"Dao Xiang","email":"","orcid":"https://orcid.org/0000-0003-1590-7193","institution":"Shanghai Jiao Tong University","correspondingAuthor":false,"prefix":"","firstName":"Dao","middleName":"","lastName":"Xiang","suffix":""}],"badges":[],"createdAt":"2025-06-19 11:11:30","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-6930601/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-6930601/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41467-026-70975-2","type":"published","date":"2026-03-19T04:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":109158102,"identity":"ec9f8ecb-c18a-4ca7-acf4-3dd250b54e18","added_by":"auto","created_at":"2026-05-13 07:08:21","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2204149,"visible":true,"origin":"","legend":"Article File","description":"","filename":"20251217maniscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6930601/v1_covered_a4da7a92-a833-42f7-b86b-df6084d4627d.pdf"},{"id":100146191,"identity":"85b2391f-e6d0-4bff-8551-83f2f5e72d1d","added_by":"auto","created_at":"2026-01-13 12:32:12","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":28823023,"visible":true,"origin":"","legend":"Supplementary information","description":"","filename":"20251217supplementaryinformation.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6930601/v1/a55d01e61feff6eec129a84d.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Noncollinear ferrielectricity in a van der Waals crystal","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-6930601/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6930601/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Inspired by noncollinear magnetic dipole order, the noncollinear electric dipole order is anticipated to induce rich ferroelectric physics for fascinating device applications. However, establishing noncollinear electric dipole ordering in single crystals is challenging due to electric polarization locking to the crystallographic axes. Here, we report the noncollinear ferrielectricity in a van der Waals crystal WO2Br2 by introducing the competition of ferroelectric and antiferroelectric modes, and uncover its critical role on the polarization switching under hydrostatic pressure and coherent phonon dynamics. The noncollinear dipole order of WO2Br2 was revealed by decoupling the antipolar displacement component along the b-axis and the polar component along the c-axis, both of which were directly visualized by scanning transmission electron microscopy (STEM). Moreover, this noncollinear dipole order not only drives the robust in-plane uniaxial macroscopic ferroelectric behavior, but also enables 90° polarization flip under hydrostatic pressure with two energetically degenerate transition pathways: one via an antipolar intermediate phase, the other through a 45° polar phase respectively. Specially, ultrafast electron diffraction measurements confirm that optical excitation drives two distinct coherent phonon modes associated with the ferroelectric and antiferroelectric orders respectively, shedding light on ultrafast control of the exotic noncollinear ferroelectric states. Our work definitely unlocks the underlying physics of noncollinear ferroelectricity for emergent ferroelectric device applications.","manuscriptTitle":"Noncollinear ferrielectricity in a van der Waals crystal","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-01-13 12:32:07","doi":"10.21203/rs.3.rs-6930601/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-communications","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"NCOMMS","sideBox":"Learn more about [Nature Communications](http://www.nature.com/ncomms/)","snPcode":"","submissionUrl":"https://mts-ncomms.nature.com/","title":"Nature Communications","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Communications","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"a54cbc30-499e-4fa3-b300-b7a51b4ef056","owner":[],"postedDate":"January 13th, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":60974298,"name":"Physical sciences/Materials science/Nanoscale materials/Two-dimensional materials"},{"id":60974299,"name":"Physical sciences/Materials science/Condensed-matter physics/Ferroelectrics and multiferroics"}],"tags":[],"updatedAt":"2026-05-13T07:07:57+00:00","versionOfRecord":{"articleIdentity":"rs-6930601","link":"https://doi.org/10.1038/s41467-026-70975-2","journal":{"identity":"nature-communications","isVorOnly":false,"title":"Nature Communications"},"publishedOn":"2026-03-19 04:00:00","publishedOnDateReadable":"March 19th, 2026"},"versionCreatedAt":"2026-01-13 12:32:07","video":"","vorDoi":"10.1038/s41467-026-70975-2","vorDoiUrl":"https://doi.org/10.1038/s41467-026-70975-2","workflowStages":[]},"version":"v1","identity":"rs-6930601","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-6930601","identity":"rs-6930601","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}