CaltechAUTHORS
Published September 27, 2021 | Version Published + Supplemental Material
Journal Article Open

The driving factors of new particle formation and growth in the polluted boundary layer

Creators

  • 1. ROR icon Paul Scherrer Institute
  • 2. ROR icon ETH Zurich
  • 3. ROR icon University of Helsinki
  • 4. ROR icon University of Vienna
  • 5. ROR icon Goethe University Frankfurt
  • 6. ROR icon Carnegie Mellon University
  • 7. ROR icon Universität Innsbruck
  • 8. ROR icon Finnish Meteorological Institute
  • 9. ROR icon University of Colorado Boulder
  • 10. ROR icon University of Lisbon
  • 11. ROR icon California Institute of Technology
  • 12. ROR icon Pusan National University
  • 13. ROR icon Peking University
  • 14. ROR icon University of Eastern Finland
  • 15. ROR icon P.N. Lebedev Physical Institute of the Russian Academy of Sciences
  • 16. ROR icon European Organization for Nuclear Research
  • 17. ROR icon Nanjing University
  • 18. ROR icon Tampere University
  • 19. ROR icon Johannes Gutenberg University of Mainz
  • 20. ROR icon University of Beira Interior
  • 21. ROR icon Aerodyne Research
  • 22. ROR icon University of Leeds
  • 23. ROR icon Beijing University of Chemical Technology

Abstract

New particle formation (NPF) is a significant source of atmospheric particles, affecting climate and air quality. Understanding the mechanisms involved in urban aerosols is important to develop effective mitigation strategies. However, NPF rates reported in the polluted boundary layer span more than 4 orders of magnitude, and the reasons behind this variability are the subject of intense scientific debate. Multiple atmospheric vapours have been postulated to participate in NPF, including sulfuric acid, ammonia, amines and organics, but their relative roles remain unclear. We investigated NPF in the CLOUD chamber using mixtures of anthropogenic vapours that simulate polluted boundary layer conditions. We demonstrate that NPF in polluted environments is largely driven by the formation of sulfuric acid–base clusters, stabilized by the presence of amines, high ammonia concentrations and lower temperatures. Aromatic oxidation products, despite their extremely low volatility, play a minor role in NPF in the chosen urban environment but can be important for particle growth and hence for the survival of newly formed particles. Our measurements quantitatively account for NPF in highly diverse urban environments and explain its large observed variability. Such quantitative information obtained under controlled laboratory conditions will help the interpretation of future ambient observations of NPF rates in polluted atmospheres.

Additional Information

© Author(s) 2021. This work is distributed under he Creative Commons Attribution 4.0 License. Received: 30 Dec 2020 – Discussion started: 20 Jan 2021 – Revised: 21 Jun 2021 – Accepted: 11 Jul 2021 – Published: 27 Sep 2021. We thank CERN for supporting CLOUD with technical and financial resources, and for providing a particle beam from the CERN Proton Synchrotron. We thank the tofTools team for providing programmes for mass spectrometry analysis. We thank Patrick Carrie, Louis-Philippe De Menezes, Ilya Krasin, Pascal Blanc, Robert Kristic, Giulio Malaguti, Osman Maksumov, Maxim Philippov, Robert Sitals and Katja Ivanova for their contributions to the experiment. This research has received funding from the following: the EC Seventh Framework Programme and the European Union's Horizon 2020 programme (Marie Skłodowska-Curie ITNs no. 316662 "CLOUD-TRAIN" and no. 764991 "CLOUD-MOTION"); Horizon 2020 Marie Skłodowska-Curie grant "Nano-CAVa" 656994 and Horizon 2020 MC-COFUND grant (665779); ERC Advanced ("ATM-GP" grant no. 227463); ERC-Consolidator Grant (NANODYNAMITE 616075); ERC-Starting grant (COALA, grant no. 638703, QAPPA, grant no. 335478); the Swiss National Science Foundation (no. 200021_169090, 200020_172602, 20FI20_ 172622); the US National Science Foundation (grant nos. AGC1439551, AGS1447056, AGS1531284, AGS1801574, AGS1801897, AGS1649147, AGS1801280, AGS1602086, 1801329); Wallace Research Foundation, German Federal Ministry of Education and Research (01LK1222A CLOUD-12 and 01LK1601A CLOUD-16); the Portuguese Foundation for Science and Technology (project no. CERN/FIS-COM/0014/2017); the Presidium of the Russian Academy of Sciences ("High energy physics and neutrino astrophysics" 2015 and the programme "Physics of Fundamental Interactions" 2017–2020); the Austrian Science Fund (FWF, project nos. J3951-N36 and P27295-N20); NASA graduate fellowship (NASA-NNX16AP36H); and the Academy of Finland (project numbers 299574, 307331, 331207, 326948, and 310682). Author contributions. MX, DS, AK, MW, HL, BM, UM, AB, MS, XCH, KL, LA, RB, DC, AD, JonD, HF, VH, CK, TK, JL CL, ZL, HM, VM, HEM, RLM, AO, EP, TP, JP, VP, LQ, MR, SieS, SimS, YS, YJT, AT, MV, AW, RW, YoW, LW, DW, Yu W, CY, PY, YY, QZ, XZ RF, MK, JK, and JosD prepared the CLOUD facility and measurement instruments. XM, CRH, LD, HL, UM, AB, TK, MR, AT, LW, AH, KC, VR, RCF, MK, DW, JK, NMD, UB, IEH, and JosD planned the experiments. MX, CRH, LD, DS, MW, HL, OG, BM, UM, AB, MS, XCH, KL, LA, RB, PSB, LB, DB, FB, SB, RC, AD, JonD, HF, VH, CK, JL, CPL, ZL, VM, RM, RLM, WN, EP, JP, VP, MR, SimS, YJT, AT, MV, AW, LW, DW, YuW, CY, PY, QY, XZ, AA, PMW, IEH, and JosD collected the data. XM, CRH, LD, DS, AK, MW, HL, OG, BM, UM, MS, HF, CK, RLM, ACW, LW, PY, RF, JosD analysed the data. XM, CRH, DS, MW, HL, OG, UM, AB, FB, HG, CK, TP, MR, SieS, PY, JC, AH, RV, RCF, KM, DW, JK, NMD, UB, IEH, and JosD contributed to the scientific discussion. MX, CRH, HL, TP, RF, NMD, UB, IEH, and JosD contributed to the writing of the paper. The supplement related to this article is available online at: https://doi.org/10.5194/acp-21-14275-2021-supplement. The authors declare that they have no conflict of interest.

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Additional details

Identifiers

Eprint ID
111468
Resolver ID
CaltechAUTHORS:20211015-162632786

Related works

Is published in
10.5194/acp-21-14275-2021-supplement (DOI)

Funding

Marie Curie Fellowship
316662
Marie Curie Fellowship
764991
Marie Curie Fellowship
656994
Marie Curie Fellowship
665779
European Research Council (ERC)
227463
European Research Council (ERC)
616075
European Research Council (ERC)
638703
European Research Council (ERC)
335478
Swiss National Science Foundation (SNSF)
200021_169090
Swiss National Science Foundation (SNSF)
200020_172602
Swiss National Science Foundation (SNSF)
20FI20_ 172622
NSF
AGC-1439551
NSF
AGS-1447056
NSF
AGS-1531284
NSF
AGS-1801574
NSF
AGS-1801897
NSF
AGS-1649147
NSF
AGS-1801280
NSF
AGS-1602086
NSF
AGS-1801329
Wallace Research Foundation
Bundesministerium für Bildung und Forschung (BMBF)
01LK1222A CLOUD-12
Bundesministerium für Bildung und Forschung (BMBF)
01LK1601A CLOUD-16
Fundação para a Ciência e a Tecnologia (FCT)
CERN/FIS-COM/0014/2017
Presidium of the Russian Academy of Sciences
FWF Der Wissenschaftsfonds
J3951-N36
FWF Der Wissenschaftsfonds
P27295-N20
NASA Graduate Fellowship
NNX16AP36H
Academy of Finland
299574
Academy of Finland
307331
Academy of Finland
331207
Academy of Finland
326948
Academy of Finland
310682

Dates

Created
2021-10-18
Created from EPrint's datestamp field
Updated
2021-10-18
Created from EPrint's last_modified field