Subshell orbital-resolved attosecond dynamics of nonadiabatic valence electrons in strong-field ionization and rescattering

Subshell orbital-resolved attosecond dynamics of nonadiabatic valence electrons in strong-field ionization and rescattering | 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 Subshell orbital-resolved attosecond dynamics of nonadiabatic valence electrons in strong-field ionization and rescattering Peng-Cheng Li, Lin Han, Jing-Jing Zhang, Sen Lan, Hong-Gang Luo This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7066917/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 Attosecond electron dynamics in strong laser fields govern fundamental light-matter interactions, yet subshell orbital-resolved ionization and rescattering processes of valence electrons have remained obscured by quantum many-body effects. Here, we present a theoretical breakthrough by combining time-dependent density functional theory (TDDFT) with Bohmian mechanics (BM) analysis (TDDFT-BM) for nonadiabatic treatment of subshell quantum-trajectory-resolved ionization and rescattering processes of many-electron atomic systems in intense laser fields, enabling attosecond-scale tracking of both ionization and rescattering dynamics in nonadiabatic multielectron systems. Angular momentum orientation-resolved BM quantum trajectories manifest an unexpected characteristic phenomenon in ionization and rescattering processes, which 3$p_{\pm1}$ electron escapes faster than 3$p_0$ and 3$s$ electrons, exhibiting an instantaneous intensity-dependent ionization delay, but a rescattering inversion occurs during photoemission, where the more deeply bound 3$s$ electrons and weakly bound 3$p_0$ electrons return to the core earlier than 3$p_{\pm1}$ electrons. This demonstrates that the orbital orientation with the electron density perpendicular to the electric field accelerates ionization but decelerates rescattering, even though the relative ionization probability is small. Our findings not only resolve long-standing puzzles in attosecond quantum dynamics but also establish TDDFT-BM as a transformative tool for controlling electronic motion at its natural timescale. Physical sciences/Optics and photonics/Optical physics/Ultrafast photonics Physical sciences/Optics and photonics/Optical physics/High-harmonic generation 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. 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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-7066917","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":508746188,"identity":"e536d8eb-c5de-4b7b-aed2-f5415526df5c","order_by":0,"name":"Peng-Cheng Li","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAArUlEQVRIiWNgGAWjYFACHsYDCRUQpgSxWhgOJJyBqCZBC2MbKVrM2c8eOPBwXl2dwQHmg7d5GOzyCGqx7MlLOJC47bCEwQG2ZGsehuRigloMbvAYALUcAGrhMZMGOjKxgTgtc+qAWvi/kaKlgRlkCxtxWix7cgwOJBw7LDnzMJux5RyDZMJazNnPGD78UVPHz3e8+eGNNxV2RDgMzmJG5RKjZRSMglEwCkYBLgAAcSY6wdx1w50AAAAASUVORK5CYII=","orcid":"https://orcid.org/0000-0002-4471-5935","institution":"Shantou University","correspondingAuthor":true,"prefix":"","firstName":"Peng-Cheng","middleName":"","lastName":"Li","suffix":""},{"id":508746189,"identity":"e17861e9-f399-492f-ae15-4ed250e3b630","order_by":1,"name":"Lin Han","email":"","orcid":"","institution":"Shantou University","correspondingAuthor":false,"prefix":"","firstName":"Lin","middleName":"","lastName":"Han","suffix":""},{"id":508746190,"identity":"bb72f0b2-5abc-48c2-aad8-264449246354","order_by":2,"name":"Jing-Jing Zhang","email":"","orcid":"","institution":"Shantou University","correspondingAuthor":false,"prefix":"","firstName":"Jing-Jing","middleName":"","lastName":"Zhang","suffix":""},{"id":508746191,"identity":"b86459cf-8874-4976-baa4-8fde1c6e8423","order_by":3,"name":"Sen Lan","email":"","orcid":"","institution":"Shantou University","correspondingAuthor":false,"prefix":"","firstName":"Sen","middleName":"","lastName":"Lan","suffix":""},{"id":508746192,"identity":"0dec5026-71cb-4adf-90a5-9b2f3c866c98","order_by":4,"name":"Hong-Gang Luo","email":"","orcid":"","institution":"Lanzhou University","correspondingAuthor":false,"prefix":"","firstName":"Hong-Gang","middleName":"","lastName":"Luo","suffix":""}],"badges":[],"createdAt":"2025-07-07 15:16:12","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-7066917/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-7066917/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":91745724,"identity":"4a297db7-7990-4a8c-ab1e-72d35b337881","added_by":"auto","created_at":"2025-09-19 22:50:04","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1767143,"visible":true,"origin":"","legend":"Article File","description":"","filename":"manuscriptLi.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7066917/v1_covered_0d14a79a-50f6-46a3-aefb-ad1dc666bf58.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Subshell orbital-resolved attosecond dynamics of nonadiabatic valence electrons in strong-field ionization and rescattering","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"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":"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-7066917/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7066917/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Attosecond electron dynamics in strong laser fields govern fundamental light-matter interactions, yet subshell orbital-resolved ionization and rescattering processes of valence electrons have remained obscured by quantum many-body effects. Here, we present a theoretical breakthrough by combining time-dependent density functional theory (TDDFT) with Bohmian mechanics (BM) analysis (TDDFT-BM) for nonadiabatic treatment of subshell quantum-trajectory-resolved ionization and rescattering processes of many-electron atomic systems in intense laser fields, enabling attosecond-scale tracking of both ionization and rescattering dynamics in nonadiabatic multielectron systems. Angular momentum orientation-resolved BM quantum trajectories manifest an unexpected characteristic phenomenon in ionization and rescattering processes, which 3$p_{\\pm1}$ electron escapes faster than 3$p_0$ and 3$s$ electrons, exhibiting an instantaneous intensity-dependent ionization delay, but a rescattering inversion occurs during photoemission, where the more deeply bound 3$s$ electrons and weakly bound 3$p_0$ electrons return to the core earlier than 3$p_{\\pm1}$ electrons. 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