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Chem. Phys."],"abstract":"<jats:p>Abstract. In the present-day atmosphere, sulfuric acid is the most\nimportant vapour for aerosol particle formation and initial growth. However,\nthe growth rates of nanoparticles (&lt;10\u2009nm) from sulfuric acid\nremain poorly measured. Therefore, the effect of stabilizing bases, the\ncontribution of ions and the impact of attractive forces on molecular\ncollisions are under debate. Here, we present precise growth rate\nmeasurements of uncharged sulfuric acid particles from 1.8 to 10\u2009nm, performed\nunder atmospheric conditions in the CERN (European\nOrganization for Nuclear Research) CLOUD chamber. Our results show\nthat the evaporation of sulfuric acid particles above 2\u2009nm is negligible,\nand growth proceeds kinetically even at low ammonia concentrations. The\nexperimental growth rates exceed the hard-sphere kinetic limit for the\ncondensation of sulfuric acid. We demonstrate that this results from\nvan der Waals forces between the vapour molecules and particles and\ndisentangle it from charge\u2013dipole interactions. The magnitude of the\nenhancement depends on the assumed particle hydration and collision\nkinetics but is increasingly important at smaller sizes, resulting in a\nsteep rise in the observed growth rates with decreasing size. Including the\nexperimental results in a global model, we find that the enhanced growth rate of\nsulfuric acid particles increases the predicted particle number concentrations\nin the upper free troposphere by more than 50\u2009%.<\/jats:p>","DOI":"10.5194\/acp-20-7359-2020","type":"journal-article","created":{"date-parts":[[2020,6,25]],"date-time":"2020-06-25T04:36:25Z","timestamp":1593059785000},"page":"7359-7372","source":"Crossref","is-referenced-by-count":85,"title":["Enhanced growth rate of atmospheric particles from sulfuric acid"],"prefix":"10.5194","volume":"20","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1014-1360","authenticated-orcid":false,"given":"Dominik","family":"Stolzenburg","sequence":"first","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4900-7460","authenticated-orcid":false,"given":"Mario","family":"Simon","sequence":"additional","affiliation":[]},{"given":"Ananth","family":"Ranjithkumar","sequence":"additional","affiliation":[]},{"given":"Andreas","family":"K\u00fcrten","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1660-2706","authenticated-orcid":false,"given":"Katrianne","family":"Lehtipalo","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1822-3224","authenticated-orcid":false,"given":"Hamish","family":"Gordon","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6517-5341","authenticated-orcid":false,"given":"Sebastian","family":"Ehrhart","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8349-3714","authenticated-orcid":false,"given":"Henning","family":"Finkenzeller","sequence":"additional","affiliation":[]},{"given":"Lukas","family":"Pichelstorfer","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2713-715X","authenticated-orcid":false,"given":"Tuomo","family":"Nieminen","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7416-306X","authenticated-orcid":false,"given":"Xu-Cheng","family":"He","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3133-249X","authenticated-orcid":false,"given":"Sophia","family":"Brilke","sequence":"additional","affiliation":[]},{"given":"Mao","family":"Xiao","sequence":"additional","affiliation":[]},{"given":"Ant\u00f3nio","family":"Amorim","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4480-2107","authenticated-orcid":false,"given":"Rima","family":"Baalbaki","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4614-247X","authenticated-orcid":false,"given":"Andrea","family":"Baccarini","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3700-5895","authenticated-orcid":false,"given":"Lisa","family":"Beck","sequence":"additional","affiliation":[]},{"given":"Steffen","family":"Br\u00e4kling","sequence":"additional","affiliation":[]},{"given":"Luc\u00eda","family":"Caudillo 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R., and Martin, S. T.: Hygroscopic growth of\nnucleation-mode acidic sulfate particles, J. Aerosol Sci., 40, 338\u2013347,\nhttps:\/\/doi.org\/10.1016\/j.jaerosci.2008.12.003, 2009.","DOI":"10.1016\/j.jaerosci.2008.12.003"},{"key":"ref2","doi-asserted-by":"crossref","unstructured":"Breitenlechner, M., Fischer, L., Hainer, M., Heinritzi, M., Curtius, J., and\nHansel, A.: PTR3: An Instrument for Studying the Lifecycle of Reactive\nOrganic Carbon in the Atmosphere, Anal. Chem., 89, 5824\u20135831,\nhttps:\/\/doi.org\/10.1021\/acs.analchem.6b05110, 2017.","DOI":"10.1021\/acs.analchem.6b05110"},{"key":"ref3","doi-asserted-by":"crossref","unstructured":"Brock, C. A., Hamill, P., Wilson, J. C., Jonsson, H. H., and Chan, K. R.:\nParticle Formation in the Upper Tropical Troposphere: A Source of Nuclei for\nthe Stratospheric Aerosol, Science, 270, 1650\u20131653,\nhttps:\/\/doi.org\/10.1126\/science.270.5242.1650, 1995.","DOI":"10.1126\/science.270.5242.1650"},{"key":"ref4","doi-asserted-by":"crossref","unstructured":"Brunelli, N. A., Flagan, R. C., and Giapis, K. P.: Radial Differential\nMobility Analyzer for One Nanometer Particle Classification, Aerosol Sci.\nTech., 43, 53\u201359, https:\/\/doi.org\/10.1080\/02786820802464302, 2009.","DOI":"10.1080\/02786820802464302"},{"key":"ref5","doi-asserted-by":"crossref","unstructured":"Bzdek, B. R., Horan, A. J., Pennington, M. R., DePalma, J. W., Zhao, J.,\nJen, C. N., Hanson, D. R., Smith, J. N., McMurry, P. H., and Johnston, M. V:\nQuantitative and time-resolved nanoparticle composition measurements during\nnew particle formation, Faraday Discuss., 165, 25\u201343,\nhttps:\/\/doi.org\/10.1039\/C3FD00039G, 2013.","DOI":"10.1039\/c3fd00039g"},{"key":"ref6","doi-asserted-by":"crossref","unstructured":"Chan, T. W. and Mozurkewich, M.: Measurement of the coagulation rate\nconstant for sulfuric acid particles as a function of particle size using\ntandem differential mobility analysis, J. Aerosol Sci., 32, 321\u2013339,\nhttps:\/\/doi.org\/10.1016\/S0021-8502(00)00081-1, 2001.","DOI":"10.1016\/S0021-8502(00)00081-1"},{"key":"ref7","doi-asserted-by":"crossref","unstructured":"Dada, L., Lehtipalo, K., Kontkanen, J., Nieminen, T., Baalbaki, R., Ahonen,\nL., Duplissy, J., Yan, C., Chu, B., Pet\u00e4j\u00e4, T., Lehtinen, K.,\nKerminen, V.-M., Kulmala, M., and Kangasluoma, J.: Formation and growth of\nsub-3-nm aerosol particles in experimental chambers, Nat. Protoc., 15, 1013\u20131040,\nhttps:\/\/doi.org\/10.1038\/s41596-019-0274-z, 2020.","DOI":"10.1038\/s41596-019-0274-z"},{"key":"ref8","doi-asserted-by":"crossref","unstructured":"Deshler, T.: A review of global stratospheric aerosol: Measurements,\nimportance, life cycle, and local stratospheric aerosol, Atmos. Res., 90,\n223\u2013232, https:\/\/doi.org\/10.1016\/j.atmosres.2008.03.016, 2008.","DOI":"10.1016\/j.atmosres.2008.03.016"},{"key":"ref9","doi-asserted-by":"crossref","unstructured":"Dunne, E. M., Gordon, H., K\u00fcrten, A., Almeida, J., Duplissy, J.,\nWilliamson, C., Ortega, I. K., Pringle, K. J., Adamov, A., Baltensperger,\nU., Barmet, P., Benduhn, F., Bianchi, F., Breitenlechner, M., Clarke, A.,\nCurtius, J., Dommen, J., Donahue, N. M., Ehrhart, S., Flagan, R. C.,\nFranchin, A., Guida, R., Hakala, J., Hansel, A., Heinritzi, M., Jokinen, T.,\nKangasluoma, J., Kirkby, J., Kulmala, M., Kupc, A., Lawler, M. J.,\nLehtipalo, K., Makhmutov, V., Mann, G., Mathot, S., Merikanto, J.,\nMiettinen, P., Nenes, A., Onnela, A., Rap, A., Reddington, C. L. S.,\nRiccobono, F., Richards, N. A. D., Rissanen, M. P., Rondo, L., Sarnela, N.,\nSchobesberger, S., Sengupta, K., Simon, M., Sipil\u00e4, M., Smith, J. N.,\nStozkhov, Y., Tom\u00e9, A., Tr\u00f6stl, J., Wagner, P. E., Wimmer, D.,\nWinkler, P. M., Worsnop, D. R., and Carslaw, K. S.: Global atmospheric\nparticle formation from CERN CLOUD measurements, Science, 354,\n1119\u20131124, https:\/\/doi.org\/10.1126\/science.aaf2649, 2016.","DOI":"10.1126\/science.aaf2649"},{"key":"ref10","doi-asserted-by":"crossref","unstructured":"Duplissy, J., Merikanto, J., Franchin, A., Tsagkogeorgas, G., Kangasluoma,\nJ., Wimmer, D., Vuollekoski, H., Schobesberger, S., Lehtipalo, K., Flagan,\nR. C., Brus, D., Donahue, N. M., Vehkam\u00e4ki, H., Almeida, J., Amorim, A.,\nBarmet, P., Bianchi, F., Breitenlechner, M., Dunne, E. 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