Crystallisation triggered by mass diffusion at a lower local supersaturation

Crystallisation triggered by mass diffusion at a lower local supersaturation | 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 Crystallisation triggered by mass diffusion at a lower local supersaturation Shuqi Xu, Juan Felipe Torres This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7305721/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 11 Feb, 2026 Read the published version in Communications Chemistry → Version 1 posted You are reading this latest preprint version Abstract Crystallisation is fundamental to many natural and industrial processes and is strongly influenced by temperature and concentration. While extensively studied under equilibrium conditions, crystallisation under non-equilibrium conditions remains less explored. Here, we demonstrate crystallisation of potassium chloride in aqueous solution driven by thermodiffusion and isothermal diffusion. The supersaturation at which crystallisation occurs is first determined through cooling crystallisation. Under thermophobic thermodiffusion, crystals formed at a lower local supersaturation compared to isothermal systems. Similarly, under isothermal diffusion between the same supersaturated solution and a lower-concentration solution, crystallisation occurred at lower concentrations and a higher temperature; thus lower local supersaturations. In particular, crystals formed in regions of the maximum concentration gradient rather than the maximum supersaturation. These findings provide macroscopic experimental evidence that non-equilibrium processes can narrow the metastable zone width, underscoring the critical role of spatial temperature and concentration control in triggering crystallisation. This work has broad implications for technologies that require precise crystallisation control. Physical sciences/Chemistry/Physical chemistry/Chemical physics Physical sciences/Chemistry/Chemical engineering Physical sciences/Chemistry/Materials chemistry Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SI.pdf Supplementary Information Cite Share Download PDF Status: Published Journal Publication published 11 Feb, 2026 Read the published version in Communications Chemistry → 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-7305721","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":500120521,"identity":"b294ff68-baed-4b18-b0c1-047d4b8f6fd8","order_by":0,"name":"Shuqi Xu","email":"","orcid":"https://orcid.org/0000-0002-2500-4951","institution":"Australian National University","correspondingAuthor":false,"prefix":"","firstName":"Shuqi","middleName":"","lastName":"Xu","suffix":""},{"id":500120520,"identity":"995ab4ca-74a6-42cc-bcc8-0572680ba4e6","order_by":1,"name":"Juan Felipe Torres","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA/klEQVRIiWNgGAWjYBAC9gbmhgMIbgWEksCnhecAI1gLVNEZIrUgFDG2EaOFvbHxcEEFQx2/9NmHD3/Os8szOMB88DYPg11iAy4tPAcbDs84wyAh2ZdubMy7LbnY4ABbsjUPQzJOLfYSiQ2HedsYJAzOsLFJM25jTtxwgMdMmoeBGbct8g+BWv6BtbD//DmnHqiF/xtQSz1uLRKMQC0NEFsYeBsOg2xhA2o5jMcvQIfNOCYhObOHjVma59jxxJmH2Ywt5xgcN8aphf3w4c8FNTb8/DxsjB9/1FQn9h1vfnjjTUW1LC4tIMCMGhHMIMIAj3qYmlEwCkbBKBgFOAEASepQpE/1zxsAAAAASUVORK5CYII=","orcid":"https://orcid.org/0000-0002-3054-8638","institution":"Australian National University","correspondingAuthor":true,"prefix":"","firstName":"Juan","middleName":"Felipe","lastName":"Torres","suffix":""}],"badges":[],"createdAt":"2025-08-06 05:05:26","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-7305721/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-7305721/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s42004-026-01925-8","type":"published","date":"2026-02-11T05:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":105039996,"identity":"ba5cf1e7-e73c-4fd1-8f10-2732a0b9211f","added_by":"auto","created_at":"2026-03-20 07:47:33","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":4776418,"visible":true,"origin":"","legend":"Article File","description":"","filename":"ms.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7305721/v1_covered_40553273-84b4-416e-a058-1d26ac2ed0ff.pdf"},{"id":89531238,"identity":"6328d762-3cfa-4257-8f24-6d131011b17d","added_by":"auto","created_at":"2025-08-21 04:04:25","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":10560855,"visible":true,"origin":"","legend":"Supplementary Information","description":"","filename":"SI.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7305721/v1/bb9f7b7eb5bfd16663eb79b6.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Crystallisation triggered by mass diffusion at a lower local supersaturation","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"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-7305721/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7305721/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Crystallisation is fundamental to many natural and industrial processes and is strongly influenced by temperature and concentration. While extensively studied under equilibrium conditions, crystallisation under non-equilibrium conditions remains less explored. Here, we demonstrate crystallisation of potassium chloride in aqueous solution driven by thermodiffusion and isothermal diffusion. The supersaturation at which crystallisation occurs is first determined through cooling crystallisation. Under thermophobic thermodiffusion, crystals formed at a lower local supersaturation compared to isothermal systems. Similarly, under isothermal diffusion between the same supersaturated solution and a lower-concentration solution, crystallisation occurred at lower concentrations and a higher temperature; thus lower local supersaturations. In particular, crystals formed in regions of the maximum concentration gradient rather than the maximum supersaturation. 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