Valence-Free Open Nanoparticle Superlattices

Valence-Free Open Nanoparticle Superlattices | 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 Valence-Free Open Nanoparticle Superlattices David Vaknin, Binay Nayak, Wenjie Wang, Prapti Kakkar, Honghu Zhang, and 5 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7256208/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 17 Jan, 2026 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract A cornerstone of next-generation materials design is establishing a framework for assembling nanoparticle superstructures with tailored symmetries. A longstanding challenge has been assembling diamond-like superstructures for photonic devices. Traditionally, such open superstructures require functionalized nanoparticles with directional or anisotropic interactions, reminiscent of valence bonding in a diamond. Here, we present a robust strategy for assembling valence-free nanoparticles into a broad array of cubic superstructures. By grafting nanoparticles with oppositely charged, end-functionalized water-soluble polymers of adjustable molecular weight, we gain control over electrostatic interactions and conformational constraints. This unified approach yields lattices analogous to rock salt, CsCl, zinc‑blende, diamond, and the exceptionally rare simple cubic phase, with tunable lattice constants. Theoretical models and simulations elucidate the underlying interactions, unlocking novel avenues for engineering valence-free nanoparticle superlattices. Physical sciences/Nanoscience and technology/Nanoscale materials/Molecular self-assembly Physical sciences/Materials science/Nanoscale materials/Metamaterials Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SI.pdf Supporting information for Valence-Free Open Nanoparticle Superlattices Cite Share Download PDF Status: Published Journal Publication published 17 Jan, 2026 Read the published version in Nature Communications → 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-7256208","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":500629835,"identity":"ade36740-5008-4862-a03d-85870124f0ba","order_by":0,"name":"David Vaknin","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAzklEQVRIie3NsQqCQBzH8b8EbuF6DtETBNfSVPoqHsK1+BBOOoVrvcjheCJ4y1Gr4JAuOfUADkHaWnS6Rdx3+i0ffgA63U9mAniwHZbBjXA8oa85gQDkEwgWBa2b9LJcxXHNuxScBHkKIqnARFZrJiXODhL801FB7HAfIRJVBisD4PMIfCy5giTtQM4uu7Z19hhDLESLnnDCSsB5/+JgEarIjfbE95kMcL6QyLNjBTEturG7yNkxIZrmnm5da/ZdvIWI4uND7mSh0+l0f98TVxFMLLoRWM8AAAAASUVORK5CYII=","orcid":"https://orcid.org/0000-0002-0899-9248","institution":"Iowa State University","correspondingAuthor":true,"prefix":"","firstName":"David","middleName":"","lastName":"Vaknin","suffix":""},{"id":500629836,"identity":"f1a36ad3-72d1-4d77-b4bc-f2a98e22ef41","order_by":1,"name":"Binay Nayak","email":"","orcid":"https://orcid.org/0000-0002-3995-4114","institution":"Iowa State University","correspondingAuthor":false,"prefix":"","firstName":"Binay","middleName":"","lastName":"Nayak","suffix":""},{"id":500629837,"identity":"43ddf572-4428-45bf-970e-ecc19120d354","order_by":2,"name":"Wenjie Wang","email":"","orcid":"","institution":"Iowa State University","correspondingAuthor":false,"prefix":"","firstName":"Wenjie","middleName":"","lastName":"Wang","suffix":""},{"id":500629838,"identity":"28befb0a-178b-4162-af5e-9fef66bb74f0","order_by":3,"name":"Prapti Kakkar","email":"","orcid":"","institution":"Iowa State University","correspondingAuthor":false,"prefix":"","firstName":"Prapti","middleName":"","lastName":"Kakkar","suffix":""},{"id":500629839,"identity":"df553216-2d96-4ceb-a02d-d0b050b8fa3e","order_by":4,"name":"Honghu Zhang","email":"","orcid":"https://orcid.org/0000-0003-1784-7825","institution":"Brookhaven National Lab","correspondingAuthor":false,"prefix":"","firstName":"Honghu","middleName":"","lastName":"Zhang","suffix":""},{"id":500629840,"identity":"89275074-75e6-4193-ba58-1f1dbbf67b21","order_by":5,"name":"Zinnia Mallick","email":"","orcid":"https://orcid.org/0009-0000-1318-5401","institution":"South Dakota School of Mines and Technology","correspondingAuthor":false,"prefix":"","firstName":"Zinnia","middleName":"","lastName":"Mallick","suffix":""},{"id":500629841,"identity":"aae6fdfe-8774-4e87-92e8-bbff99b99178","order_by":6,"name":"Shan Zhou","email":"","orcid":"https://orcid.org/0000-0002-6476-3280","institution":"South Dakota School of Mines and Technology","correspondingAuthor":false,"prefix":"","firstName":"Shan","middleName":"","lastName":"Zhou","suffix":""},{"id":500629842,"identity":"2f38dbc0-22b8-4353-bd68-9eb54c49fa79","order_by":7,"name":"Dmytro Nykypanchuk","email":"","orcid":"","institution":"Brookhaven National Laboratory","correspondingAuthor":false,"prefix":"","firstName":"Dmytro","middleName":"","lastName":"Nykypanchuk","suffix":""},{"id":500629843,"identity":"20e1af08-f87e-4e75-b246-9e8609ca48e4","order_by":8,"name":"Surya Mallapragada","email":"","orcid":"https://orcid.org/0000-0002-9482-7273","institution":"Iowa State University","correspondingAuthor":false,"prefix":"","firstName":"Surya","middleName":"","lastName":"Mallapragada","suffix":""},{"id":500629844,"identity":"11315d60-b4a7-4105-9337-7922bde5f214","order_by":9,"name":"Alex Travesset","email":"","orcid":"","institution":"Iowa State University","correspondingAuthor":false,"prefix":"","firstName":"Alex","middleName":"","lastName":"Travesset","suffix":""}],"badges":[],"createdAt":"2025-07-30 20:30:16","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-7256208/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-7256208/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41467-026-68316-4","type":"published","date":"2026-01-17T05:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":102654441,"identity":"40ec0d7e-49ca-4d7a-b844-edbd0dd5784b","added_by":"auto","created_at":"2026-02-14 08:06:45","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":5611024,"visible":true,"origin":"","legend":"Article File","description":"","filename":"Main.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7256208/v1_covered_36c515f3-f515-4167-8f69-05a97f59ded5.pdf"},{"id":89292913,"identity":"4ab35583-c475-473e-bc3f-55e69546f2a5","added_by":"auto","created_at":"2025-08-18 12:46:21","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":18181398,"visible":true,"origin":"","legend":"Supporting information for Valence-Free Open Nanoparticle Superlattices","description":"","filename":"SI.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7256208/v1/e13f6affc2c07fa336668f4a.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Valence-Free Open Nanoparticle Superlattices","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-7256208/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7256208/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"A cornerstone of next-generation materials design is establishing a framework for assembling nanoparticle superstructures with tailored symmetries. A longstanding challenge has been assembling diamond-like superstructures for photonic devices. Traditionally, such open superstructures require functionalized nanoparticles with directional or anisotropic interactions, reminiscent of valence bonding in a diamond. Here, we present a robust strategy for assembling valence-free nanoparticles into a broad array of cubic superstructures. By grafting nanoparticles with oppositely charged, end-functionalized water-soluble polymers of adjustable molecular weight, we gain control over electrostatic interactions and conformational constraints. This unified approach yields lattices analogous to rock salt, CsCl, zinc‑blende, diamond, and the exceptionally rare simple cubic phase, with tunable lattice constants. Theoretical models and simulations elucidate the underlying interactions, unlocking novel avenues for engineering valence-free nanoparticle superlattices.","manuscriptTitle":"Valence-Free Open Nanoparticle Superlattices","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-08-18 12:46:16","doi":"10.21203/rs.3.rs-7256208/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-communications","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"NCOMMS","sideBox":"Learn more about [Nature Communications](http://www.nature.com/ncomms/)","snPcode":"","submissionUrl":"https://mts-ncomms.nature.com/","title":"Nature Communications","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Communications","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"d1daea75-d633-4b98-9f49-0517690cc188","owner":[],"postedDate":"August 18th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":53186153,"name":"Physical sciences/Nanoscience and technology/Nanoscale materials/Molecular self-assembly"},{"id":53186154,"name":"Physical sciences/Materials science/Nanoscale materials/Metamaterials"}],"tags":[],"updatedAt":"2026-02-14T08:06:34+00:00","versionOfRecord":{"articleIdentity":"rs-7256208","link":"https://doi.org/10.1038/s41467-026-68316-4","journal":{"identity":"nature-communications","isVorOnly":false,"title":"Nature Communications"},"publishedOn":"2026-01-17 05:00:00","publishedOnDateReadable":"January 17th, 2026"},"versionCreatedAt":"2025-08-18 12:46:16","video":"","vorDoi":"10.1038/s41467-026-68316-4","vorDoiUrl":"https://doi.org/10.1038/s41467-026-68316-4","workflowStages":[]},"version":"v1","identity":"rs-7256208","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7256208","identity":"rs-7256208","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}