Coalescence of water droplets at 125 K

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Abstract In spite of four decades of research on vitrified glassy water droplets, their flow properties in the deeply supercooled regime below 160 K have remained elusive. However, they are key to astrophysical processes where molecules are transported between water interfaces in the deeply supercooled or glassy state. Here we observe coalescence of a deposit consisting of thousands of micrometer-sized glassy water droplets between ~123 and ~140 K. Both electron microscopy and small-angle X-ray scattering indicate the disappearance of droplet interfaces at the time scale of minutes. Scattering profiles suggest a mechanism involving stretching of droplets and confluence. Remarkably, these phenomena coincide with water’s first glass transition, which thus defines the verge between glassy and liquid water. This marks the observation of coalescence in the ultraviscous domain, whereas previously coalescence has only been recognized for temperatures above 260 K, at which viscosity is thirteen orders of magnitude lower. Our findings indicate a recoupling of viscosity to translational diffusion below 160 K, while decoupling and breakdown of the Stokes-Einstein relation take place above 250 K. Coalescence under cryoconditions might take place in grainy amorphous ice covering interstellar dust particles in molecular clouds, enabling the formation of complex molecules in space.
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Coalescence of water droplets at 125 K | 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 Coalescence of water droplets at 125 K Thomas Loerting, Johannes Giebelmann, Tobias Eklund, Ulrike Boesenberg, and 19 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-5112004/v2 This work is licensed under a CC BY 4.0 License Status: Posted Version 2 posted You are reading this latest preprint version Show more versions Abstract In spite of four decades of research on vitrified glassy water droplets, their flow properties in the deeply supercooled regime below 160 K have remained elusive. However, they are key to astrophysical processes where molecules are transported between water interfaces in the deeply supercooled or glassy state. Here we observe coalescence of a deposit consisting of thousands of micrometer-sized glassy water droplets between ~123 and ~140 K. Both electron microscopy and small-angle X-ray scattering indicate the disappearance of droplet interfaces at the time scale of minutes. Scattering profiles suggest a mechanism involving stretching of droplets and confluence. Remarkably, these phenomena coincide with water’s first glass transition, which thus defines the verge between glassy and liquid water. This marks the observation of coalescence in the ultraviscous domain, whereas previously coalescence has only been recognized for temperatures above 260 K, at which viscosity is thirteen orders of magnitude lower. Our findings indicate a recoupling of viscosity to translational diffusion below 160 K, while decoupling and breakdown of the Stokes-Einstein relation take place above 250 K. Coalescence under cryoconditions might take place in grainy amorphous ice covering interstellar dust particles in molecular clouds, enabling the formation of complex molecules in space. Physical sciences/Physics/Condensed-matter physics Physical sciences/Physics/Chemical physics Full Text Additional Declarations There is NO Competing Interest. Supplementary Files Rawdataguide.txt Raw Data Guide GiebelmannnatphysSI.docx Supplementary Information MovieS1.mp4 Movie S1 Cite Share Download PDF Status: Posted Version 2 posted You are reading this latest preprint version Show more versions 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. 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