Spontaneous and self-oriented growth during chemical vapor epitaxy of single-crystalline MoS2

Spontaneous and self-oriented growth during chemical vapor epitaxy of single-crystalline MoS2 | 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 Spontaneous and self-oriented growth during chemical vapor epitaxy of single-crystalline MoS 2 Annelies Delabie, Iryna Kandybka, Pawan Kumar, Henry Medina, Benjamin Groven, and 8 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7114151/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Conventional chemical vapor epitaxy concepts for single-crystalline molybdenum disulfide (MoS 2 ) rely on sapphire template engineering to impart a preferred crystalline orientation. However, such epitaxy concepts may fall short to curb within-wafer statistical variance of the MoS 2 crystal orientation when manufacturing sapphire substrates to semiconductor industry-standard specifications and wafer size. Here, we report metal-organic chemical vapor epitaxy of single-crystalline MoS 2 without sapphire template engineering. By lowering the metal-organic precursor adsorption rate in the mass-transport-limited reaction regime, the MoS 2 nucleation and growth rate slows down sufficiently for spontaneous and self-oriented MoS 2 growth to proceed. During this self-oriented growth, the bulk sapphire crystallographic symmetry governs the MoS 2 epitaxial registry, rather than the surface structure and termination of the sapphire steps and terraces. Even though 60°-oriented MoS 2 twin crystals deposit, a single-crystalline MoS 2 monolayer forms by annihilating the mirror twin grain boundaries through spontaneous van der Waals recrystallization during and after the coalescence of the MoS 2 monolayer. We show a proof of concept in a 300 mm industrial pilot-line, yielding median carrier mobilities up to 30 ± 5 cm 2 V –1 s –1 . Crucially, self-oriented growth alleviates the stringent requirements to pertain to a critically low and saturated areal density of MoS 2 crystals, to develop unidirectional crystal orientation during the initial growth regime, or to minimize sapphire surface anomalies from substrate manufacturing. Hence, van der Waals recrystallization presents a vital mechanism during chemical vapor epitaxy to further modulate crystal defect structures in various transition metal dichalcogenides and substrates compatible with both bonding-to-wafer and monolithic integration approaches. Physical sciences/Nanoscience and technology/Nanoscale materials/Two-dimensional materials Physical sciences/Materials science/Nanoscale materials/Synthesis and processing Full Text Additional Declarations There is NO Competing Interest. Supplementary Files Supplementary1307.pdf Supplementary information Cite Share Download PDF Status: Posted 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-7114151","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":494911930,"identity":"9bf0393d-e1d8-4649-876e-5d612ed31ffe","order_by":0,"name":"Annelies 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MoS\u003csub\u003e2\u003c/sub\u003e","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-7114151/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7114151/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Conventional chemical vapor epitaxy concepts for single-crystalline molybdenum disulfide (MoS\u003csub\u003e2\u003c/sub\u003e) rely on sapphire template engineering to impart a preferred crystalline orientation. However, such epitaxy concepts may fall short to curb within-wafer statistical variance of the MoS\u003csub\u003e2\u003c/sub\u003e crystal orientation when manufacturing sapphire substrates to semiconductor industry-standard specifications and wafer size. Here, we report metal-organic chemical vapor epitaxy of single-crystalline MoS\u003csub\u003e2\u003c/sub\u003e without sapphire template engineering. By lowering the metal-organic precursor adsorption rate in the mass-transport-limited reaction regime, the MoS\u003csub\u003e2\u003c/sub\u003e nucleation and growth rate slows down sufficiently for spontaneous and self-oriented MoS\u003csub\u003e2\u003c/sub\u003e growth to proceed. During this self-oriented growth, the bulk sapphire crystallographic symmetry governs the MoS\u003csub\u003e2\u003c/sub\u003e epitaxial registry, rather than the surface structure and termination of the sapphire steps and terraces. Even though 60°-oriented MoS\u003csub\u003e2\u003c/sub\u003e twin crystals deposit, a single-crystalline MoS\u003csub\u003e2\u003c/sub\u003e monolayer forms by annihilating the mirror twin grain boundaries through spontaneous van der Waals recrystallization during and after the coalescence of the MoS\u003csub\u003e2\u003c/sub\u003e monolayer. We show a proof of concept in a 300 mm industrial pilot-line, yielding median carrier mobilities up to 30 ± 5 cm\u003csup\u003e2\u003c/sup\u003eV\u003csup\u003e–1\u003c/sup\u003es\u003csup\u003e–1\u003c/sup\u003e. Crucially, self-oriented growth alleviates the stringent requirements to pertain to a critically low and saturated areal density of MoS\u003csub\u003e2\u003c/sub\u003e crystals, to develop unidirectional crystal orientation during the initial growth regime, or to minimize sapphire surface anomalies from substrate manufacturing. Hence, van der Waals recrystallization presents a vital mechanism during chemical vapor epitaxy to further modulate crystal defect structures in various transition metal dichalcogenides and substrates compatible with both bonding-to-wafer and monolithic integration approaches.","manuscriptTitle":"Spontaneous and self-oriented growth during chemical vapor epitaxy of single-crystalline MoS2","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-08-05 02:58:07","doi":"10.21203/rs.3.rs-7114151/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"2a0baba8-58b0-45e3-b903-1c4b4b02d08f","owner":[],"postedDate":"August 5th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":52558928,"name":"Physical sciences/Nanoscience and technology/Nanoscale materials/Two-dimensional materials"},{"id":52558929,"name":"Physical sciences/Materials science/Nanoscale materials/Synthesis and processing"}],"tags":[],"updatedAt":"2025-12-29T08:20:29+00:00","versionOfRecord":[],"versionCreatedAt":"2025-08-05 02:58:07","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-7114151","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7114151","identity":"rs-7114151","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}