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Enhanced growth rate of atmospheric particles from sulfuric acid
Enhanced growth rate of atmospheric particles from sulfuric acid
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 %.
- Goethe University Frankfurt Germany
- Hebei University China (People's Republic of)
- Max Planck Society Germany
- Max Planck Institute for Heart and Lung Research Germany
- University of Colorado Boulder United States
6817
Biskos, G., Buseck, P. R., and Martin, S. T.: Hygroscopic growth of nucleation-mode acidic sulfate particles, J. Aerosol Sci., 40, 338-347, https://doi.org/10.1016/j.jaerosci.2008.12.003, 2009.
Breitenlechner, M., Fischer, L., Hainer, M., Heinritzi, M., Curtius, J., and Hansel, A.: PTR3: An Instrument for Studying the Lifecycle of Reactive Organic Carbon in the Atmosphere, Anal. Chem., 89, 5824-5831, https://doi.org/10.1021/acs.analchem.6b05110, 2017.
Brock, C. A., Hamill, P., Wilson, J. C., Jonsson, H. H., and Chan, K. R.: Particle Formation in the Upper Tropical Troposphere: A Source of Nuclei for the Stratospheric Aerosol, Science, 270, 1650-1653, https://doi.org/10.1126/science.270.5242.1650, 1995.
Brunelli, N. A., Flagan, R. C., and Giapis, K. P.: Radial Differential Mobility Analyzer for One Nanometer Particle Classification, Aerosol Sci. Tech., 43, 53-59, https://doi.org/10.1080/02786820802464302, 2009.
Bzdek, B. R., Horan, A. J., Pennington, M. R., DePalma, J. W., Zhao, J., Jen, C. N., Hanson, D. R., Smith, J. N., McMurry, P. H., and Johnston, M. V: Quantitative and time-resolved nanoparticle composition measurements during new particle formation, Faraday Discuss., 165, 25-43, https://doi.org/10.1039/C3FD00039G, 2013.
Chan, T. W. and Mozurkewich, M.: Measurement of the coagulation rate constant for sulfuric acid particles as a function of particle size using tandem differential mobility analysis, J. Aerosol Sci., 32, 321-339, https://doi.org/10.1016/S0021- 8502(00)00081-1, 2001. [OpenAIRE]
Dada, L., Lehtipalo, K., Kontkanen, J., Nieminen, T., Baalbaki, R., Ahonen, L., Duplissy, J., Yan, C., Chu, B., Petäjä, T., Lehtinen, K., Kerminen, V.-M., Kulmala, M., and Kangasluoma, J.: Formation and growth of sub-3-nm aerosol particles in experimental chambers, Nat. Protoc., 15, 1013-1040, https://doi.org/10.1038/s41596-019-0274-z, 2020. [OpenAIRE]
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Dunne, E. M., Gordon, H., Kürten, A., Almeida, J., Duplissy, J., Williamson, C., Ortega, I. K., Pringle, K. J., Adamov, A., Baltensperger, U., Barmet, P., Benduhn, F., Bianchi, F., Breitenlechner, M., Clarke, A., Curtius, J., Dommen, J., Donahue, N. M., Ehrhart, S., Flagan, R. C., Franchin, A., Guida, R., Hakala, J., Hansel, A., Heinritzi, M., Jokinen, T., Kangasluoma, J., Kirkby, J., Kulmala, M., Kupc, A., Lawler, M. J., Lehtipalo, K., Makhmutov, V., Mann, G., Mathot, S., Merikanto, J., Miettinen, P., Nenes, A., Onnela, A., Rap, A., Reddington, C. L. S., Riccobono, F., Richards, N. A. D., Rissanen, M. P., Rondo, L., Sarnela, N., Schobesberger, S., Sengupta, K., Simon, M., Sipilä, M., Smith, J. N., Stozkhov, Y., Tomé, A., Tröstl, J., Wagner, P. E., Wimmer, D., Winkler, P. M., Worsnop, D. R., and Carslaw, K. S.: Global atmospheric particle formation from CERN CLOUD measurements, Science, 354, 1119-1124, https://doi.org/10.1126/science.aaf2649, 2016.
Duplissy, J., Merikanto, J., Franchin, A., Tsagkogeorgas, G., Kangasluoma, J., Wimmer, D., Vuollekoski, H., Schobesberger, S., Lehtipalo, K., Flagan, R. C., Brus, D., Donahue, N. M., Vehkamäki, H., Almeida, J., Amorim, A., Barmet, P., Bianchi, F., Breitenlechner, M., Dunne, E. M., Guida, R., Henschel, H., Junninen, H., Kirkby, J., Kürten, A., Kupc, A., Määttänen, A., Makhmutov, V., Mathot, S., Nieminen, T., Onnela, A., Praplan, A. P., Riccobono, F., Rondo, L., Steiner, G., Tome, A., Walther, H., Baltensperger, U., Carslaw, K. S., Dommen, J., Hansel, A., Petäjä, T., Sipilä, M., Stratmann, F., Vrtala, A., Wagner, P. E., Worsnop, D. R., Curtius, J., and Kulmala, M.: Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory, J. Geophys. Res.-Atmos., 121, 1752-1775, https://doi.org/10.1002/2015JD023539, 2016. [OpenAIRE]
citations This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).0 popularity This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.Average influence This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).Average impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.Average citations This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).0 popularity This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.Average influence This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).Average impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.Average
Popularity provided by BIP!- Swiss National Science Foundation (SNSF)
- 159851
- Infrastructure | Research Infrastructure
- Austrian Science Fund (FWF) (FWF)
- P 27295
- Einzelprojekte
- National Science Foundation (NSF)
- 1801280
- Directorate for Geosciences | Division of Atmospheric and Geospace Sciences
- Goethe University Frankfurt Germany
- Hebei University China (People's Republic of)
- Max Planck Society Germany
- Max Planck Institute for Heart and Lung Research Germany
- University of Colorado Boulder United States
- California Institute of Technology United States
- University of Vienna Austria
- Carnegie Mellon University United States
- Tampere University Finland
- Carnegie-Mellon University United States
- Nanjing University China (People's Republic of)
- Pusan National University
- European Organization for Nuclear Research Switzerland
- Divis. of Chemistry and Chemical Engineering California Inst. of Techn. United States
- Center for Atmospheric Particle Studies Carnegie Mellon University United States
- Labor für Atmosphärenchemie Paul Scherrer Institut Switzerland
- Finnish Meteorological Institute Finland
- JOHANN WOLFGANG GOETHE UNIVERSITAET FRANKFURT AM MAIN Germany
- University of Innsbruck, Institute for Ion Physics and Applied Physics Austria
- TOFWERK AG Switzerland
- Paul Scherrer Institute Switzerland
- Universität Innsbruck Austria
- University of Helsinki Finland
- Universidade de Lisboa Instituto Dom Luiz
- Kunsan National University Korea (Republic of)
- University of Leeds United Kingdom
- Max Planck Institute for Chemistry Germany
- Paul Scherrer Institute Switzerland
- Institute for atmoaspheric and earth system research (INAR) University of Helsinki Finland
- Universidade da Beira Interior
- Division of Chemistry and Chemical Engineering California Institute of Technology United States
- Goethe University Frankfurt Germany
- Nanjing University China (People's Republic of)
- Div. of Chemistry and Chemical Engineering California Institute of Technology United States
- Institut f. Ionenphysik und Angewandte Physik Universität Innsbruck
- Ionicon Analytik (Austria) Austria
- University of Beira Interior Portugal
- University of Eastern Finland Finland
- Pusan National University Korea (Republic of)
- P.N. Lebedev Physical Institute of the Russian Academy of Sciences Russian Federation
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 %.