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The transformation of amorphous Ca-, Ca\u2013Mg-, and Mg-carbonate (ACC, ACMC, and AMC) phases is sensitive to relative humidity (RH) of the surrounding air. Here, we measure the effective thicknesses of water films on amorphous carbonates from 10 to 98% RH using a dynamic vapor sorption analyzer and specific surface areas from N2 adsorption. We find that water sorption increases exponentially starting at 76\u201384% RH for ACMC phases (21 \u2264 mol % Mg \u2264 100). We supplement these data with static sorption experiments at 98% RH and constrain sorption rates and effective equilibrium water film thicknesses to 2\u20136 nm. In long-term experiments with fixed humidity, ACMC and its transformation products show evidence of continued recrystallization over a period of seven months at 98% RH. Diverse crystal morphologies suggest distinct microenvironments of recrystallization. Finally, recrystallization of mixed Ca\u2013Mg-carbonate phases to discrete Ca- and Mg-carbonate minerals suggests a process of ion transport in the thin films. We discuss how Ostwald ripening, phase metastability, and ion diffusion may operate as drivers of recrystallization in thin film environments.<\/jats:p>","DOI":"10.1021\/acs.cgd.6c00090","type":"journal-article","created":{"date-parts":[[2026,6,9]],"date-time":"2026-06-09T08:10:18Z","timestamp":1780992618000},"page":"6282-6295","source":"Crossref","is-referenced-by-count":0,"title":["Dissolution\u2013Reprecipitation of Amorphous and\nCrystalline (Ca)\u2013Mg-Carbonates in Thin Water Films"],"prefix":"10.1021","volume":"26","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2126-561X","authenticated-orcid":true,"given":"Avni S.","family":"Patel","sequence":"first","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 2E3"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Maija J.","family":"Raudsepp","sequence":"additional","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 2E3"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jean-Michel","family":"Brazier","sequence":"additional","affiliation":[{"name":"University of Bern , , ,","place":["Bern, Switzerland, 3012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Anna L.","family":"Harrison","sequence":"additional","affiliation":[{"name":"University of Bern , , ,","place":["Bern, Switzerland, 3012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0858-6902","authenticated-orcid":true,"given":"Sasha","family":"Wilson","sequence":"additional","affiliation":[{"name":"University of Alberta , , , ,","place":["Edmonton, Alberta, Canada, T6G 2E3"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,6,9]]},"reference":[{"issue":"6247","key":"2026081909110428000_cit1","doi-asserted-by":"publisher","first-page":"aaa6760","DOI":"10.1126\/science.aaa6760","article-title":"Crystallization\nby Particle Attachment in Synthetic, Biogenic, and Geologic Environments","volume":"349","author":"De Yoreo","year":"2015","journal-title":"Science"},{"issue":"16","key":"2026081909110428000_cit2","doi-asserted-by":"publisher","first-page":"6088","DOI":"10.1073\/pnas.1118085109","article-title":"Phase Transitions in Biogenic Amorphous\nCalcium Carbonate","volume":"109","author":"Gong","year":"2012","journal-title":"Proc. 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Geochem."},{"issue":"11","key":"2026081909110428000_cit6","doi-asserted-by":"publisher","first-page":"6663","DOI":"10.1021\/acs.cgd.6b00794","article-title":"A Review of Classical and Nonclassical\nNucleation Theories","volume":"16","author":"Karthika","year":"2016","journal-title":"Cryst. Growth Des."},{"issue":"29","key":"2026081909110428000_cit7","doi-asserted-by":"publisher","first-page":"16983","DOI":"10.1021\/acs.jpcc.8b05189","article-title":"Role of Impurities\nin the Kinetic Persistence of Amorphous\nCalcium Carbonate: A Nanoscopic Dynamics View","volume":"122","author":"Koishi","year":"2018","journal-title":"J. Phys. Chem. C"},{"issue":"6","key":"2026081909110428000_cit8","doi-asserted-by":"publisher","first-page":"1900002","DOI":"10.1002\/crat.201900002","article-title":"Effect of\nStrontium Ions on Crystallization of Amorphous Calcium Carbonate","volume":"54","author":"Schmidt","year":"2019","journal-title":"Cryst. Res. 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Crystallogr."},{"issue":"6","key":"2026081909110428000_cit29","doi-asserted-by":"publisher","first-page":"911","DOI":"10.1107\/s0021889804022551","article-title":"Size-Strain Line-Broadening\nAnalysis of the Ceria Round-Robin Sample","volume":"37","author":"Balzar","year":"2004","journal-title":"J.\nAppl. Crystallogr."},{"issue":"4","key":"2026081909110428000_cit30","doi-asserted-by":"publisher","first-page":"278","DOI":"10.1154\/1.2362855","article-title":"Quantification of Phases with Partial\nor No Known Crystal\nStructures","volume":"21","author":"Scarlett","year":"2006","journal-title":"Powder Diffr."},{"issue":"2","key":"2026081909110428000_cit31","doi-asserted-by":"publisher","first-page":"309","DOI":"10.1021\/ja01269a023","article-title":"Adsorption of Gases in Multimolecular\nLayers","volume":"60","author":"Brunauer","year":"1938","journal-title":"J. Am. Chem. Soc."},{"issue":"1","key":"2026081909110428000_cit32","doi-asserted-by":"publisher","DOI":"10.1002\/vzj2.20063","article-title":"Changes in\nWater Vapor Adsorption and Water Film Thickness in Clayey Materials\nas a Function of Relative Humidity","volume":"19","author":"Lin","year":"2020","journal-title":"Vadose Zone\nJ."},{"issue":"17","key":"2026081909110428000_cit33","doi-asserted-by":"publisher","first-page":"L99","DOI":"10.1016\/j.susc.2009.06.021","article-title":"Calcite (1014) surface\nin humid environments","volume":"603","author":"Baltrusaitis","year":"2009","journal-title":"Surf. Sci."},{"key":"2026081909110428000_cit34","doi-asserted-by":"publisher","first-page":"5985","DOI":"10.1016\/j.gca.2010.08.003","article-title":"Thickness and\nStructure of the Water Film Deposited from Vapour on Calcite Surfaces","volume":"74","author":"Bohr","year":"2010","journal-title":"Geochem. Cosmochim. Acta"},{"key":"2026081909110428000_cit35","doi-asserted-by":"publisher","first-page":"W08514","DOI":"10.1029\/2011WR010676","article-title":"Physicochemical\nControls on Adsorbed Water Film Thickness in Unsaturated Geological\nMedia","volume":"47","author":"Tokunaga","year":"2011","journal-title":"Water Resour. Res."},{"key":"2026081909110428000_cit36","doi-asserted-by":"publisher","first-page":"32136","DOI":"10.1038\/srep32136","article-title":"Particle Size Controls on Water Adsorption and Condensation\nRegimes at Mineral Surfaces","volume":"6","author":"Yes\u0327ilbas\u0327","year":"2016","journal-title":"Sci. Rep."},{"issue":"8","key":"2026081909110428000_cit37","doi-asserted-by":"publisher","first-page":"4338","DOI":"10.1021\/acs.est.6b05891","article-title":"Ion Diffusion Within Water Films in Unsaturated Porous\nMedia","volume":"51","author":"Tokunaga","year":"2017","journal-title":"Environ. Sci. Technol."},{"issue":"4","key":"2026081909110428000_cit38","doi-asserted-by":"publisher","first-page":"281","DOI":"10.1080\/02786820802047115","article-title":"Water Uptake\nby NaCl Particles Prior to Deliquescence and the Phase Rule","volume":"42","author":"Wise","year":"2008","journal-title":"Aerosol Sci. Technol."},{"key":"2026081909110428000_cit39","doi-asserted-by":"publisher","first-page":"7874","DOI":"10.1021\/ic8007409","article-title":"On the Structure\nof\nAmorphous Calcium Carbonate\u2500A Detailed Study by Solid-State\nNMR Spectroscopy","volume":"47","author":"Nebel","year":"2008","journal-title":"Inorg. Chem."},{"issue":"3\u20134","key":"2026081909110428000_cit40","doi-asserted-by":"publisher","first-page":"63","DOI":"10.1016\/j.pcrysgrow.2014.09.005","article-title":"Surface Properties of Biomimetic\nNanocrystalline Apatites; Applications in Biomaterials","volume":"60","author":"Rey","year":"2014","journal-title":"Prog. Cryst. Growth Charact. Mater."},{"issue":"4","key":"2026081909110428000_cit41","doi-asserted-by":"publisher","first-page":"1016","DOI":"10.1039\/B918849E","article-title":"Controlling Crystal\nGrowth with Modifiers","volume":"12","author":"Jones","year":"2010","journal-title":"CrystEngComm"},{"issue":"1","key":"2026081909110428000_cit42","doi-asserted-by":"publisher","first-page":"219","DOI":"10.1016\/j.jcrysgro.2007.01.032","article-title":"Control of\nCrystal Morphology through Supersaturation\nRatio and Mixing Conditions","volume":"304","author":"Li","year":"2007","journal-title":"J. Cryst. Growth"},{"issue":"3","key":"2026081909110428000_cit43","doi-asserted-by":"publisher","first-page":"505","DOI":"10.1021\/jp0647129","article-title":"Water-Induced Reconstruction\nthat Affects Mobile Ions\non the Surface of Calcite","volume":"111","author":"Kendall","year":"2007","journal-title":"J. Phys. Chem. A"},{"issue":"1","key":"2026081909110428000_cit44","doi-asserted-by":"publisher","first-page":"87","DOI":"10.2138\/rmg.2009.70.3","article-title":"Mineral Replacement\nReactions","volume":"70","author":"Putnis","year":"2009","journal-title":"Rev. Mineral. Geochem."},{"issue":"33","key":"2026081909110428000_cit45","doi-asserted-by":"publisher","first-page":"12096","DOI":"10.1073\/pnas.0404778101","article-title":"Energetic\nClues to Pathways to Biomineralization: Precursors, Clusters, and\nNanoparticles","volume":"101","author":"Navrotsky","year":"2004","journal-title":"Proc. Natl. Acad. Sci. U.S.A."},{"issue":"24","key":"2026081909110428000_cit46","doi-asserted-by":"publisher","first-page":"5768","DOI":"10.1021\/j150668a002","article-title":"The Ostwald Step Rule","volume":"88","author":"Van Santen","year":"1984","journal-title":"J. Phys.\nChem."},{"key":"2026081909110428000_cit47","first-page":"385","article-title":"Blocking\nof Ostwald Ripening Allowing Long-Term Stabilization","volume":"37","author":"Ostwald","year":"1901","journal-title":"Z. Phys. Chem."},{"key":"2026081909110428000_cit48","doi-asserted-by":"publisher","first-page":"369","DOI":"10.1016\/j.gca.2022.06.041","article-title":"Rates of Carbon\nand Oxygen Isotope Exchange between Calcite and Fluid at Chemical\nEquilibrium","volume":"335","author":"Harrison","year":"2022","journal-title":"Geochim. Cosmochim. Acta"},{"key":"2026081909110428000_cit49","doi-asserted-by":"publisher","first-page":"258","DOI":"10.1016\/j.gca.2020.02.032","article-title":"Oxygen and\nClumped Isotope Fractionation during the Formation of Mg Calcite via\nan Amorphous Precursor","volume":"276","author":"Dietzel","year":"2020","journal-title":"Geochim. Cosmochim.\nActa"},{"key":"2026081909110428000_cit50","doi-asserted-by":"publisher","first-page":"227","DOI":"10.1016\/j.svgl.2017.01.031","article-title":"Impact of Amorphous Precursor Phases on Magnesium Isotope\nSignatures of Mg-Calcite","volume":"464","author":"Mavromatis","year":"2017","journal-title":"Earth Planet. Sci.\nLett."},{"issue":"8","key":"2026081909110428000_cit51","doi-asserted-by":"publisher","first-page":"4385","DOI":"10.1021\/acs.cgd.9b00179","article-title":"Tuning the\nIncorporation of Magnesium into Calcite\nduring Its Crystallization from Additive-Free Aqueous Solution","volume":"19","author":"Xto","year":"2019","journal-title":"Cryst. Growth Des."},{"issue":"44","key":"2026081909110428000_cit52","doi-asserted-by":"publisher","first-page":"15491","DOI":"10.1021\/la303410w","article-title":"Self-Generated Diffusioosmotic Flows from Calcium Carbonate\nMicropumps","volume":"28","author":"McDermott","year":"2012","journal-title":"Langmuir"},{"issue":"21","key":"2026081909110428000_cit53","doi-asserted-by":"publisher","first-page":"4686","DOI":"10.1039\/C6SM00052E","article-title":"Origins of\nConcentration Gradients for Diffusiophoresis","volume":"12","author":"Velegol","year":"2016","journal-title":"Soft Matter"},{"issue":"3","key":"2026081909110428000_cit54","doi-asserted-by":"publisher","first-page":"1346","DOI":"10.1021\/cr8003828","article-title":"Effect of\nIons on the Structure of Water: Structure Making and Breaking","volume":"109","author":"Marcus","year":"2009","journal-title":"Chem. Rev."},{"key":"2026081909110428000_cit55","doi-asserted-by":"publisher","first-page":"477","DOI":"10.1016\/j.gca.2014.10.020","article-title":"Influence of Surface\nPassivation and Water Content on Mineral Reactions in Unsaturated\nPorous Media: Implications for Brucite Carbonation and CO2 Sequestration","volume":"148","author":"Harrison","year":"2015","journal-title":"Geochim. Cosmochim. Acta"},{"key":"2026081909110428000_cit56","doi-asserted-by":"publisher","first-page":"65","DOI":"10.1016\/j.chemgeo.2015.12.005","article-title":"The Impact of Evolving\nMineral-Water-Gas Interfacial Areas on Mineral-Fluid Reaction Rates\nin Unsaturated Porous Media","volume":"421","author":"Harrison","year":"2016","journal-title":"Chem. Geol."}],"container-title":["Crystal Growth &amp; Design"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/acs.cgd.6c00090","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/cgdefu\/article-pdf\/26\/16\/6282\/66257090\/acs.cgd.6c00090.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/cgdefu\/article-pdf\/26\/16\/6282\/66257090\/acs.cgd.6c00090.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,8,19]],"date-time":"2026-08-19T13:22:53Z","timestamp":1787145773000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/cgdefu\/article\/26\/16\/6282\/5232475\/Dissolution-Reprecipitation-of-Amorphous-and"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,6,9]]},"references-count":56,"journal-issue":{"issue":"16","published-online":{"date-parts":[[2026,6,9]]},"published-print":{"date-parts":[[2026,8,19]]}},"URL":"https:\/\/doi.org\/10.1021\/acs.cgd.6c00090","relation":{},"ISSN":["1528-7483","1528-7505"],"issn-type":[{"value":"1528-7483","type":"print"},{"value":"1528-7505","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,6,9]]}}}