Atomic-Scale Engineering of d-π-d Spin Interaction in Metal-Organic Architectures

Atomic-Scale Engineering of d-π-d Spin Interaction in Metal-Organic Architectures | 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 Atomic-Scale Engineering of d-π-d Spin Interaction in Metal-Organic Architectures Yongfeng Wang, Xue Zhang, Xin Li, Jie Li, Haoyang Pan, Minghui Yu, and 14 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7151282/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 Spin coupling between magnetic metal atoms and organic radicals plays a pivotal role in high-performance magnetic materials. The complex interaction involving multi-spin centers in bulk materials makes it challenging to study spin coupling at the atomic scale. Here, we investigate the d-π-d spin interaction in well-defined metal-organic coordinated structures composed of two iron (Fe) atoms and four all-trans retinoic acid (ReA) molecules, using low-temperature scanning tunneling microscopy and atomic force microscopy. The ReA molecule is turned into a spin-1/2 radical state by dehydrogenation, facilitating strong magnetic coupling with the coordinated Fe atoms. Comprehensive theoretical analysis, based on density functional theory and valence bond theory, further elucidates the intrinsic mechanism of ferrimagnetic spin coupling in the coordination structure. Specifically, simultaneous antiferromagnetic coupling of Fe dimer to ReA radicals parallelizes the dimer spin orientation. This work contributes to the fundamental understanding of spin interaction in metal-organic coordination structures and provides microscopic insights for designing advanced magnetic materials. Physical sciences/Chemistry/Surface chemistry/Scanning probe microscopy Physical sciences/Chemistry/Physical chemistry Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SI2025dpdcoupling.docx Supplemental Materials for Atomic-Scale Engineering of d-π-d Spin Interaction in Metal-Organic Architectures 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. 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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-7151282","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":489154116,"identity":"0bc80729-cb85-411f-965f-5d7b40e35893","order_by":0,"name":"Yongfeng 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