CaltechAUTHORS
Published June 25, 2020 | Version Published + Supplemental Material
Journal Article Open

Enhanced growth rate of atmospheric particles from sulfuric acid

Creators

  • 1. ROR icon University of Vienna
  • 2. ROR icon University of Helsinki
  • 3. ROR icon Goethe University Frankfurt
  • 4. ROR icon University of Leeds
  • 5. ROR icon Finnish Meteorological Institute
  • 6. ROR icon Max Planck Institute for Chemistry
  • 7. ROR icon University of Colorado Boulder
  • 8. ROR icon Paul Scherrer Institute
  • 9. ROR icon University of Lisbon
  • 10. ROR icon Tofwerk (Switzerland)
  • 11. ROR icon Carnegie Mellon University
  • 12. ROR icon Universität Innsbruck
  • 13. ROR icon California Institute of Technology
  • 14. ROR icon Pusan National University
  • 15. ROR icon Ionicon Analytik (Austria)
  • 16. ROR icon University of Eastern Finland
  • 17. ROR icon P.N. Lebedev Physical Institute of the Russian Academy of Sciences
  • 18. ROR icon European Organization for Nuclear Research
  • 19. ROR icon Nanjing University
  • 20. ROR icon Tampere University
  • 21. ROR icon University of Beira Interior

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 %.

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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Additional details

Identifiers

Eprint ID
104425
Resolver ID
CaltechAUTHORS:20200717-102144160

Related works

Is published in
10.5194/acp-20-7359-2020-supplement (DOI)

Funding

CERN
Marie Curie Fellowship
764991
Marie Curie Fellowship
665779
European Research Council (ERC)
616075
European Research Council (ERC)
714621
Bundesministerium für Bildung und Forschung (BMBF)
01LK1601A
Swiss National Science Foundation (SNSF)
200020_152907
Swiss National Science Foundation (SNSF)
20FI20_159851
Swiss National Science Foundation (SNSF)
200021_169090
Swiss National Science Foundation (SNSF)
200020_172602
Swiss National Science Foundation (SNSF)
20FI20_172622
Academy of Finland
296628
Academy of Finland
299574
Academy of Finland
307331
Academy of Finland
310682
FWF Der Wissenschaftsfonds
J-3951
FWF Der Wissenschaftsfonds
P27295-N20
FWF Der Wissenschaftsfonds
J-4241
Fundação para a Ciência e a Tecnologia (FCT)
CERN/FIS-COM/0014/2017
NSF
AGS-1649147
NSF
AGS-1801280
NSF
AGS-1602086
NSF
AGS-1801329
University of Vienna

Dates

Created
2020-07-17
Created from EPrint's datestamp field
Updated
2021-11-16
Created from EPrint's last_modified field