Impedance microscopy for imaging solid-state battery interfaces

Impedance microscopy for imaging solid-state battery interfaces | 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 Impedance microscopy for imaging solid-state battery interfaces Yuji Yamagishi, Hirotada Gamo, Zyun Siroma, Naoya Ishida, Yasushi Maeda, and 4 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9468966/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 Electrochemical impedance spectroscopy (EIS) is widely used to probe interfaces in solid-state electrochemical devices, including all-solid-state batteries (ASSBs). However, its lack of spatial resolution has long hindered unambiguous identification of the origins of individual impedance components. Here we introduce electrochemical impedance spectroscopy–atomic force microscopy (EIS-AFM), an AFM-based platform for impedance analysis with simultaneous frequency and nanoscale spatial resolution. By enabling AC voltage distribution mapping with an AFM probe over an ultra-wide frequency range (0.1 Hz–1 MHz), EIS-AFM covers most frequencies used in EIS-based battery analysis and enables spatially resolved impedance mapping within ASSBs. Applied to sulfide-based ASSBs, EIS-AFM quantifies the interfacial impedance between the alloy anode and the sulfide solid electrolyte and reveals that high-voltage degradation of LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM) cathodes proceeds as a coupled process involving resistive interphase growth at the cathode/electrolyte interface and concurrent formation of locally high-impedance grain boundaries within NCM particles. EIS-AFM provides a general platform for nanoscale impedance imaging. Physical sciences/Materials science/Techniques and instrumentation/Microscopy/Atomic force microscopy Physical sciences/Nanoscience and technology/Techniques and instrumentation/Microscopy/Scanning probe microscopy Physical sciences/Energy science and technology/Energy storage/Batteries Physical sciences/Materials science/Materials for energy and catalysis/Batteries Physical sciences/Chemistry/Electrochemistry/Batteries Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SI.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-9468966","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":635456347,"identity":"1869df20-4a15-4273-a338-683ae1823d5e","order_by":0,"name":"Yuji Yamagishi","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA/ElEQVRIiWNgGAWjYBADHgYJxsYHDAZQrgSRWpoNgFokiNYCUsUmQZRigwM8hp9u1NTKyM9ubqv4UVBXx8C/+ACD5Q68Woylc44d5zG4c7DtZo/BYQkGiWcJDJJn8GoxkM5hO8ZjIJHYdoPH4ABQyxkDBsk2/Lb8zvl3jEd+RmJb4R+DOqK0mEnnttXwMNxIbGPmMWCWYODvwa9F8jBbmXVuH9B5NxKbpWUMDku2SbAlHMDnF77jzZtv53yrs5efkf7w45s/dfz8/IcPPpbEE2IKhzlAMX4YIcImkcBwWLIBtxb5BvYHQKoOSYj/AAPjRzxaRsEoGAWjYMQBAHeCTzVO/MuoAAAAAElFTkSuQmCC","orcid":"https://orcid.org/0000-0001-6269-2426","institution":"National Institute of Advanced Industrial Science and Technology (AIST)","correspondingAuthor":true,"prefix":"","firstName":"Yuji","middleName":"","lastName":"Yamagishi","suffix":""},{"id":635456349,"identity":"461c5327-1c69-48dd-b178-8cba2e14e915","order_by":1,"name":"Hirotada Gamo","email":"","orcid":"https://orcid.org/0000-0002-5817-9985","institution":"National Institute of Advanced Industrial Science and Technology (AIST)","correspondingAuthor":false,"prefix":"","firstName":"Hirotada","middleName":"","lastName":"Gamo","suffix":""},{"id":635456350,"identity":"24b3557c-6733-413a-a227-543afb08389a","order_by":2,"name":"Zyun Siroma","email":"","orcid":"","institution":"National Institute of Advanced Industrial Science and Technology (AIST)","correspondingAuthor":false,"prefix":"","firstName":"Zyun","middleName":"","lastName":"Siroma","suffix":""},{"id":635456352,"identity":"fd3e55f0-1d02-462c-8290-341c3c78fe70","order_by":3,"name":"Naoya Ishida","email":"","orcid":"","institution":"National Institute of Advanced Industrial Science and Technology (AIST)","correspondingAuthor":false,"prefix":"","firstName":"Naoya","middleName":"","lastName":"Ishida","suffix":""},{"id":635456353,"identity":"47a4ab6a-7451-4f27-b278-f06dfcda25e1","order_by":4,"name":"Yasushi Maeda","email":"","orcid":"","institution":"National Institute of Advanced Industrial Science and Technology (AIST)","correspondingAuthor":false,"prefix":"","firstName":"Yasushi","middleName":"","lastName":"Maeda","suffix":""},{"id":635456355,"identity":"475609ca-363c-4e79-a765-e3c29d3668f8","order_by":5,"name":"Tetsu Kiyobayashi","email":"","orcid":"","institution":"National Institute of Advanced Industrial Science and Technology (AIST)","correspondingAuthor":false,"prefix":"","firstName":"Tetsu","middleName":"","lastName":"Kiyobayashi","suffix":""},{"id":635456356,"identity":"08f99738-1088-4427-a1f9-fbbb038469e8","order_by":6,"name":"Nobuhiko Takeichi","email":"","orcid":"","institution":"National Institute of Advanced Industrial Science and Technology (AIST)","correspondingAuthor":false,"prefix":"","firstName":"Nobuhiko","middleName":"","lastName":"Takeichi","suffix":""},{"id":635456358,"identity":"371edc95-0fe3-4295-b556-e4623a324383","order_by":7,"name":"Kentaro Kuratani","email":"","orcid":"","institution":"National Institute of Advanced Industrial Science and Technology (AIST)","correspondingAuthor":false,"prefix":"","firstName":"Kentaro","middleName":"","lastName":"Kuratani","suffix":""},{"id":635456361,"identity":"8ff27ecc-f365-427b-8cfc-9058ba2cbb38","order_by":8,"name":"Hikaru Sano","email":"","orcid":"https://orcid.org/0000-0002-7557-0767","institution":"National Institute of Advanced Industrial Science and Technology (AIST)","correspondingAuthor":false,"prefix":"","firstName":"Hikaru","middleName":"","lastName":"Sano","suffix":""}],"badges":[],"createdAt":"2026-04-20 08:22:56","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-9468966/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-9468966/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":109296523,"identity":"c08552cc-5915-4b80-8628-b90c3598fb18","added_by":"auto","created_at":"2026-05-15 08:47:49","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1147496,"visible":true,"origin":"","legend":"Article File","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-9468966/v1_covered_da6edd07-404f-423c-ae31-eea62a0c2bbf.pdf"},{"id":109289593,"identity":"b9cb7d27-528c-4c8a-a281-b53cc7049a2c","added_by":"auto","created_at":"2026-05-15 06:31:56","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":1433113,"visible":true,"origin":"","legend":"Supplementary Information","description":"","filename":"SI.pdf","url":"https://assets-eu.researchsquare.com/files/rs-9468966/v1/9362c632bf626c74dc364e1a.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Impedance microscopy for imaging solid-state battery interfaces","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-9468966/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-9468966/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Electrochemical impedance spectroscopy (EIS) is widely used to probe interfaces in solid-state electrochemical devices, including all-solid-state batteries (ASSBs). However, its lack of spatial resolution has long hindered unambiguous identification of the origins of individual impedance components. Here we introduce electrochemical impedance spectroscopy–atomic force microscopy (EIS-AFM), an AFM-based platform for impedance analysis with simultaneous frequency and nanoscale spatial resolution. By enabling AC voltage distribution mapping with an AFM probe over an ultra-wide frequency range (0.1 Hz–1 MHz), EIS-AFM covers most frequencies used in EIS-based battery analysis and enables spatially resolved impedance mapping within ASSBs. Applied to sulfide-based ASSBs, EIS-AFM quantifies the interfacial impedance between the alloy anode and the sulfide solid electrolyte and reveals that high-voltage degradation of LiNi\u003csub\u003e0.5\u003c/sub\u003eCo\u003csub\u003e0.2\u003c/sub\u003eMn\u003csub\u003e0.3\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e (NCM) cathodes proceeds as a coupled process involving resistive interphase growth at the cathode/electrolyte interface and concurrent formation of locally high-impedance grain boundaries within NCM particles. EIS-AFM provides a general platform for nanoscale impedance imaging.","manuscriptTitle":"Impedance microscopy for imaging solid-state battery interfaces","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-05-15 06:31:53","doi":"10.21203/rs.3.rs-9468966/v1","editorialEvents":[],"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":"e036b1c1-4d28-4aaa-9157-a859afbf0d2b","owner":[],"postedDate":"May 15th, 2026","published":true,"recentEditorialEvents":[{"type":"editorAssigned","content":"","date":"2026-05-06T11:30:36+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2026-05-01T11:52:39+00:00","index":"","fulltext":""},{"type":"submitted","content":"Nature Communications","date":"2026-05-01T00:26:36+00:00","index":"","fulltext":""}],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":67629706,"name":"Physical sciences/Materials science/Techniques and instrumentation/Microscopy/Atomic force microscopy"},{"id":67629707,"name":"Physical sciences/Nanoscience and technology/Techniques and instrumentation/Microscopy/Scanning probe microscopy"},{"id":67629709,"name":"Physical sciences/Energy science and technology/Energy storage/Batteries"},{"id":67629710,"name":"Physical sciences/Materials science/Materials for energy and catalysis/Batteries"},{"id":67629712,"name":"Physical sciences/Chemistry/Electrochemistry/Batteries"}],"tags":[],"updatedAt":"2026-05-15T06:31:53+00:00","versionOfRecord":[],"versionCreatedAt":"2026-05-15 06:31:53","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-9468966","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-9468966","identity":"rs-9468966","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}