Stolzenburg, Dominik and Simon, Mario and Ranjithkumar, Ananth and Kürten, Andreas and Lehtipalo, Katrianne and Gordon, Hamish and Ehrhart, Sebastian and Finkenzeller, Henning and Pichelstorfer, Lukas and Nieminen, Tuomo and He, Xu-Cheng and Brilke, Sophia and Xiao, Mao and Amorim, António and Baalbaki, Rima and Baccarini, Andrea and Beck, Lisa and Bräkling, Steffen and Caudillo Murillo, Lucía and Chen, Dexian and Chu, Biwu and Dada, Lubna and Dias, António and Dommen, Josef and Duplissy, Jonathan and El Haddad, Imad and Fischer, Lukas and Gonzalez Carracedo, Loic and Heinritzi, Martin and Kim, Changhyuk and Koenig, Theodore K. and Kong, Weimeng and Lamkaddam, Houssni and Lee, Chuan Ping and Leiminger, Markus and Li, Zijun and Makhmutov, Vladimir and Manninen, Hanna E. and Marie, Guillaume and Marten, Ruby and Müller, Tatjana and Nie, Wei and Partoll, Eva and Petäjä, Tuukka and Pfeifer, Joschka and Philippov, Maxim and Rissanen, Matti P. and Rörup, Birte and Schobesberger, Siegfried and Schuchmann, Simone and Shen, Jiali and Sipilä, Mikko and Steiner, Gerhard and Stozhkov, Yuri and Tauber, Christian and Tham, Yee Jun and Tomé, António and Vazquez-Pufleau, Miguel and Wagner, Andrea C. and Wang, Mingyi and Wang, Yonghong and Weber, Stefan K. and Wimmer, Daniela and Wlasits, Peter J. and Wu, Yusheng and Ye, Qing and Zauner-Wieczorek, Marcel and Baltensperger, Urs and Carslaw, Kenneth S. and Curtius, Joachim and Donahue, Neil M. and Flagan, Richard C. and Hansel, Armin and Kulmala, Markku and Lelieveld, Jos and Volkamer, Rainer and Kirkby, Jasper and Winkler, Paul M. (2020) Enhanced growth rate of atmospheric particles from sulfuric acid. Atmospheric Chemistry and Physics, 20 (12). pp. 7359-7372. ISSN 1680-7324. https://resolver.caltech.edu/CaltechAUTHORS:20200717-102144160
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Abstract
In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles (<10 nm) from sulfuric acid remain poorly measured. Therefore, the effect of stabilizing bases, the contribution of ions and the impact of attractive forces on molecular collisions are under debate. Here, we present precise growth rate measurements of uncharged sulfuric acid particles from 1.8 to 10 nm, performed under atmospheric conditions in the CERN (European Organization for Nuclear Research) CLOUD chamber. Our results show that the evaporation of sulfuric acid particles above 2 nm is negligible, and growth proceeds kinetically even at low ammonia concentrations. The experimental growth rates exceed the hard-sphere kinetic limit for the condensation of sulfuric acid. We demonstrate that this results from van der Waals forces between the vapour molecules and particles and disentangle it from charge–dipole interactions. The magnitude of the enhancement depends on the assumed particle hydration and collision kinetics but is increasingly important at smaller sizes, resulting in a steep rise in the observed growth rates with decreasing size. Including the experimental results in a global model, we find that the enhanced growth rate of sulfuric acid particles increases the predicted particle number concentrations in the upper free troposphere by more than 50 %.
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| Additional Information: | © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License. Published by Copernicus Publications on behalf of the European Geosciences Union. Received: 22 August 2019 – Discussion started: 15 November 2019. Revised: 12 May 2020 – Accepted: 31 May 2020 – Published: 25 June 2020. We thank CERN for supporting CLOUD with technical and financial resources and for providing a particle beam from the CERN Proton Synchrotron. We are also grateful to Patrick Carrie, Louis-Philippe De Menezes, Jonathan Dumollard, Katja Ivanova, Francisco Josa, Timo Keber, Ilia Krasin, Robert Kristic, Abdelmajid Laassiri, Osman Maksumov, Benjamin Marichy, Herve Martinati, Robert Sitals, Albin Wasem, Sergey Vitaljevich Mizin and Mats Wilhelmsson for their contributions to the experiment. Data availability: All of the datasets presented in this paper are available from the corresponding author upon reasonable request. The supplement related to this article is available online at: https://doi.org/10.5194/acp-20-7359-2020-supplement. Author contributions: DS, MSim, AK, KL, HF, XH, SBri, MX, RB, AB, SBrä, LCM, DC, BC, AD, JDo, JDu, IEH, LF, LGC, MH, CK, WK, HL, CPL, ML, ZL, VM, HEM, TM, EP, JP, MP, MPR, SScho, SSchu, JS, MSip, GS, YS, YJT, AT, ACW, MW, YW, SKW, DW, PJW, YW, QY, MZW, UB, JC, RCF, RV, JK and PMW prepared the CLOUD facility or measuring instruments. DS, MSim, AR, KL, XH, SBri, MX, AA, RB, AB, LB, SBrä, LCM, DC, LD, AD, JDu, IEH, HF, LF, LGC, MH, CK, TKK, WK, HL, CPL, ML, ZL, HEM, RM, TM, WN, EP, JP, MPR, BR, SSchu, GS, CT, YJT, AT, MVP, ACW, MW, SKW, DW, PJW, YW, QY and MZW collected the data. DS, MSim, AR, HG, TN, LP, LD, HF, SE, MH, CK, ACW and SKW analysed the data. DS, MS, AR, AK, KL, TN, XH, MX, JDo, JDu, IEH, TKK, TP, MPR, MSip, UB, KSC, JC, NMD, RCF, AH, MK, JL, RV, JK and PMW were involved in the scientific discussion and the interpretation of the data. DS, AK, KL, HG, NMD, JK and PMW wrote the paper. The authors declare that they have no conflict of interest. This article is part of the special issue “The CERN CLOUD experiment (ACP/AMT inter-journal SI)”. It is not associated with a conference. This research has received funding from the European Commission Seventh Framework Programme and the European Union's Horizon 2020 programme (Marie Skłodowska-Curie action no. 764991 “CLOUD-MOTION”; MC-COFUND grant no. 665779 and ERC projects nos. 616075 “NANODYNAMITE” and 714621 “GASPARCON”), the German Federal Ministry of Education and Research (grant no. 01LK1601A “CLOUD-16”), the Swiss National Science Foundation (project nos. 200020_152907, 20FI20_159851, 200021_169090, 200020_172602 and 20FI20_172622), the Academy of Finland (project nos. 296628, 299574, 307331 and 310682), the Austrian Science Fund (FWF; project nos. J-3951, P27295-N20 and J-4241), the Portuguese Foundation for Science and Technology (FCT; project no. CERN/FIS-COM/0014/2017), the U.S. National Science Foundation (grant nos. AGS-1649147, AGS-1801280, AGS-1602086 and AGS-1801329). Open access funding was provided by University of Vienna. Review statement: This paper was edited by Jonathan Abbatt and reviewed by David R. Hanson and two anonymous referees. | ||||||||||||||||||||||||||||||||||||||||||||||||||
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| Issue or Number: | 12 | ||||||||||||||||||||||||||||||||||||||||||||||||||
| Record Number: | CaltechAUTHORS:20200717-102144160 | ||||||||||||||||||||||||||||||||||||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20200717-102144160 | ||||||||||||||||||||||||||||||||||||||||||||||||||
| Official Citation: | Stolzenburg, D., Simon, M., Ranjithkumar, A., Kürten, A., Lehtipalo, K., Gordon, H., Ehrhart, S., Finkenzeller, H., Pichelstorfer, L., Nieminen, T., He, X.-C., Brilke, S., Xiao, M., Amorim, A., Baalbaki, R., Baccarini, A., Beck, L., Bräkling, S., Caudillo Murillo, L., Chen, D., Chu, B., Dada, L., Dias, A., Dommen, J., Duplissy, J., El Haddad, I., Fischer, L., Gonzalez Carracedo, L., Heinritzi, M., Kim, C., Koenig, T. K., Kong, W., Lamkaddam, H., Lee, C. P., Leiminger, M., Li, Z., Makhmutov, V., Manninen, H. E., Marie, G., Marten, R., Müller, T., Nie, W., Partoll, E., Petäjä, T., Pfeifer, J., Philippov, M., Rissanen, M. P., Rörup, B., Schobesberger, S., Schuchmann, S., Shen, J., Sipilä, M., Steiner, G., Stozhkov, Y., Tauber, C., Tham, Y. J., Tomé, A., Vazquez-Pufleau, M., Wagner, A. C., Wang, M., Wang, Y., Weber, S. K., Wimmer, D., Wlasits, P. J., Wu, Y., Ye, Q., Zauner-Wieczorek, M., Baltensperger, U., Carslaw, K. S., Curtius, J., Donahue, N. M., Flagan, R. C., Hansel, A., Kulmala, M., Lelieveld, J., Volkamer, R., Kirkby, J., and Winkler, P. M.: Enhanced growth rate of atmospheric particles from sulfuric acid, Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, 2020 | ||||||||||||||||||||||||||||||||||||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||||||||||||||||||||||||||||||||||
| ID Code: | 104425 | ||||||||||||||||||||||||||||||||||||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||||||||||||||||||||||||||||||||||||
| Deposited By: | Tony Diaz | ||||||||||||||||||||||||||||||||||||||||||||||||||
| Deposited On: | 17 Jul 2020 17:51 | ||||||||||||||||||||||||||||||||||||||||||||||||||
| Last Modified: | 17 Jul 2020 17:51 |
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