Atomic-scale visualisation of interfacial degradation in halide perovskites via multidimensional in-situ electron microscopy

Atomic-scale visualisation of interfacial degradation in halide perovskites via multidimensional in-situ electron microscopy | 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 Physical Sciences - Article Atomic-scale visualisation of interfacial degradation in halide perovskites via multidimensional in-situ electron microscopy Caterina Ducati This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6692602/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 11 Mar, 2026 Read the published version in Nature → Version 1 posted You are reading this latest preprint version Abstract Halide perovskite light-emitting diodes (PeLEDs) promise high-efficiency, low-cost optoelectronics, yet their operational instability remains a critical barrier to practical deployment. Here, we develop a multimodal in-situ electron microscopy approach that integrates four-dimensional scanning transmission electron microscopy (4D-STEM), energy-dispersive X-ray spectroscopy (EDS), and atomic-resolution imaging to directly visualize structural and chemical evolution in a working PeLED with nanometre precision. Our in-situ biasing measurements uncover nanoscale structural and chemical transformations initiated at transport layer interfaces, including the formation of metallic lead and lead-rich secondary phases, as well as strain-driven grain fragmentation. Upon biasing, we observe the partial transformation of the metallic Al contact to insulating AlCl₃. Crucially, while the perovskite emitter’s bulk remains relatively intact, our experiment shows that degradation is localized at interfaces. By comparing in-situ and ex-situ measurements, these results establish a mechanistic link between interfacial strain, ionic transport, and electrochemical reactions in working devices, and provide a broadly applicable framework for nanoscale degradation analysis in complex multilayered optoelectronic systems using multimodal in-situ biasing microscopy. Physical sciences/Nanoscience and technology/Nanoscale devices/Electronic devices Physical sciences/Materials science/Techniques and instrumentation/Characterization and analytical techniques Physical sciences/Nanoscience and technology/Nanoscale materials/Organic–inorganic nanostructures Full Text Additional Declarations There is NO Competing Interest. Supplementary Files InsitubiasingPeLEDSI.pdf Atomic-scale visualisation of interfacial degradation in halide perovskites via multidimensional in-situ electron microscopy Cite Share Download PDF Status: Published Journal Publication published 11 Mar, 2026 Read the published version in Nature → 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-6692602","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Physical Sciences - Article","associatedPublications":[],"authors":[{"id":463754673,"identity":"f3aeb236-bb3f-4a6d-8e91-b819d52719d8","order_by":0,"name":"Caterina Ducati","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAt0lEQVRIiWNgGAWjYFCC5OMfEirgvARitKSlMTw4Q5qWHDPGh22kaOFvTzB7kDjPTl63gfnhB8a2NMJaJM48SDdI3JZsuO0Am7EEY1sOYS0GEgkHJBK3HWDcdoDBjIGxrYIYLYkNEolzDthvO8D+jVgtyWxAXQeAFvGAbCHCYRJnnjEbJBxLTt52mKdYIuEcEd7nb8//+PBHjZ3ttuPtGz98KEsmrAUBmBmIjMhRMApGwSgYBYQBAB+SOncH36n/AAAAAElFTkSuQmCC","orcid":"https://orcid.org/0000-0003-3366-6442","institution":"University of Cambridge","correspondingAuthor":true,"prefix":"","firstName":"Caterina","middleName":"","lastName":"Ducati","suffix":""}],"badges":[],"createdAt":"2025-05-18 15:25:19","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-6692602/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-6692602/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41586-026-10238-8","type":"published","date":"2026-03-11T04:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":104487542,"identity":"aa0e27bf-2e03-4e39-9d4c-b5e1fb3df784","added_by":"auto","created_at":"2026-03-12 10:46:23","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1385076,"visible":true,"origin":"","legend":"Article File","description":"","filename":"InsitubiasingPeLEDMaintext.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6692602/v1_covered_96405dc0-3864-4299-8018-37f0a0fbfa9a.pdf"},{"id":83660103,"identity":"360a4505-8c83-417a-97fc-fb23a4da943c","added_by":"auto","created_at":"2025-05-30 09:42:32","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":2897683,"visible":true,"origin":"","legend":"Atomic-scale visualisation of interfacial degradation in halide perovskites via multidimensional in-situ electron microscopy","description":"","filename":"InsitubiasingPeLEDSI.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6692602/v1/b4ad15febb3b8ebd2eac2093.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Atomic-scale visualisation of interfacial degradation in halide perovskites via multidimensional in-situ electron microscopy","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-6692602/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6692602/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Halide perovskite light-emitting diodes (PeLEDs) promise high-efficiency, low-cost optoelectronics, yet their operational instability remains a critical barrier to practical deployment. 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