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

Xiao, Mao and Hoyle, Christopher R. and Dada, Lubna and Stolzenburg, Dominik and Kürten, Andreas and Wang, Mingyi and Lamkaddam, Houssni and Garmash, Olga and Mentler, Bernhard and Molteni, Ugo and Baccarini, Andrea and Simon, Mario and He, Xu-Cheng and Lehtipalo, Katrianne and Ahonen, Lauri R. and Baalbaki, Rima and Bauer, Paulus S. and Beck, Lisa and Bell, David and Bianchi, Federico and Brilke, Sophia and Chen, Dexian and Chiu, Randall and Dias, António and Duplissy, Jonathan and Finkenzeller, Henning and Gordon, Hamish and Hofbauer, Victoria and Kim, Changhyuk and Koenig, Theodore K. and Lampilahti, Janne and Lee, Chuan Ping and Li, Zijun and Mai, Huajun and Makhmutov, Vladimir and Manninen, Hanna E. and Marten, Ruby and Mathot, Serge and Mauldin, Roy L. and Nie, Wei and Onnela, Antti and Partoll, Eva and Petäjä, Tuukka and Pfeifer, Joschka and Pospisilova, Veronika and Quéléver, Lauriane L. J. and Rissanen, Matti and Schobesberger, Siegfried and Schuchmann, Simone and Stozhkov, Yuri and Tauber, Christian and Tham, Yee Jun and Tomé, António and Vazquez-Pufleau, Miguel and Wagner, Andrea C. and Wagner, Robert and Wang, Yonghong and Weitz, Lena and Wimmer, Daniela and Wu, Yusheng and Yan, Chao and Ye, Penglin and Ye, Qing and Zha, Qiaozhi and Zhou, Xueqin and Amorim, Antonio and Carslaw, Ken and Curtius, Joachim and Hansel, Armin and Volkamer, Rainer and Winkler, Paul M. and Flagan, Richard C. and Kulmala, Markku and Worsnop, Douglas R. and Kirkby, Jasper and Donahue, Neil M. and Baltensperger, Urs and El Haddad, Imad and Dommen, Josef (2021) The driving factors of new particle formation and growth in the polluted boundary layer. Atmospheric Chemistry and Physics, 21 (18). pp. 14275-14291. ISSN 1680-7324. doi:10.5194/acp-21-14275-2021. https://resolver.caltech.edu/CaltechAUTHORS:20211015-162632786

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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.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.5194/acp-21-14275-2021DOIArticle
https://doi.org/10.5194/acp-21-14275-2021-supplementPublisherSupporting Information
ORCID:
AuthorORCID
Xiao, Mao0000-0002-2790-4443
Hoyle, Christopher R.0000-0002-1369-9143
Dada, Lubna0000-0003-1105-9043
Stolzenburg, Dominik0000-0003-1014-1360
Kürten, Andreas0000-0002-8955-4450
Wang, Mingyi0000-0001-5782-2513
Lamkaddam, Houssni0000-0001-5166-6353
Garmash, Olga0000-0002-9675-3271
Mentler, Bernhard0000-0003-3852-0397
Molteni, Ugo0000-0002-1623-1933
Baccarini, Andrea0000-0003-4614-247X
Simon, Mario0000-0002-4900-7460
He, Xu-Cheng0000-0002-7416-306X
Lehtipalo, Katrianne0000-0002-1660-2706
Ahonen, Lauri R.0000-0002-2534-6898
Baalbaki, Rima0000-0002-4480-2107
Bauer, Paulus S.0000-0002-0014-3082
Beck, Lisa0000-0003-3700-5895
Bell, David0000-0002-3958-2138
Bianchi, Federico0000-0003-2996-3604
Brilke, Sophia0000-0003-3133-249X
Chen, Dexian0000-0001-6963-5205
Chiu, Randall0000-0002-9892-2761
Dias, António0000-0002-0842-4639
Duplissy, Jonathan0000-0001-8819-0264
Finkenzeller, Henning0000-0002-8349-3714
Gordon, Hamish0000-0002-1822-3224
Hofbauer, Victoria0000-0001-9036-4446
Kim, Changhyuk0000-0002-8744-4880
Koenig, Theodore K.0000-0002-3756-4315
Lee, Chuan Ping0000-0003-0051-8179
Li, Zijun0000-0002-2973-1216
Mai, Huajun0000-0002-0616-1986
Makhmutov, Vladimir0000-0002-2242-1055
Manninen, Hanna E.0000-0002-0419-4020
Marten, Ruby0000-0003-0417-4350
Mauldin, Roy L.0000-0002-8569-8561
Nie, Wei0000-0002-6048-0515
Onnela, Antti0000-0001-9946-9762
Petäjä, Tuukka0000-0002-1881-9044
Pfeifer, Joschka0000-0002-9172-4447
Pospisilova, Veronika0000-0003-2559-2252
Quéléver, Lauriane L. J.0000-0001-8970-3594
Rissanen, Matti0000-0003-0463-8098
Schobesberger, Siegfried0000-0002-5777-4897
Stozhkov, Yuri0000-0003-1917-0328
Tauber, Christian0000-0003-1453-1067
Tham, Yee Jun0000-0001-7924-5841
Tomé, António0000-0001-9144-7120
Vazquez-Pufleau, Miguel0000-0001-6836-5098
Wagner, Andrea C.0000-0003-3159-9434
Wagner, Robert0000-0001-7365-8020
Wang, Yonghong0000-0003-2498-9143
Wimmer, Daniela0000-0002-5539-9958
Yan, Chao0000-0002-5735-9597
Ye, Penglin0000-0002-6954-4028
Ye, Qing0000-0003-3797-8988
Zha, Qiaozhi0000-0001-6301-7086
Amorim, Antonio0000-0003-0638-2321
Carslaw, Ken0000-0002-6800-154X
Curtius, Joachim0000-0003-3153-4630
Hansel, Armin0000-0002-1062-2394
Volkamer, Rainer0000-0002-0899-1369
Winkler, Paul M.0000-0001-6861-6029
Flagan, Richard C.0000-0001-5690-770X
Kulmala, Markku0000-0003-3464-7825
Worsnop, Douglas R.0000-0002-8928-8017
Kirkby, Jasper0000-0003-2341-9069
Donahue, Neil M.0000-0003-3054-2364
Baltensperger, Urs0000-0003-0079-8713
El Haddad, Imad0000-0002-2461-7238
Dommen, Josef0000-0002-0006-0009
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.
Funders:
Funding AgencyGrant Number
Marie Curie Fellowship316662
Marie Curie Fellowship764991
Marie Curie Fellowship656994
Marie Curie Fellowship665779
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
NSFAGC-1439551
NSFAGS-1447056
NSFAGS-1531284
NSFAGS-1801574
NSFAGS-1801897
NSFAGS-1649147
NSFAGS-1801280
NSFAGS-1602086
NSFAGS-1801329
Wallace Research FoundationUNSPECIFIED
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 SciencesUNSPECIFIED
FWF Der WissenschaftsfondsJ3951-N36
FWF Der WissenschaftsfondsP27295-N20
NASA Graduate FellowshipNNX16AP36H
Academy of Finland299574
Academy of Finland307331
Academy of Finland331207
Academy of Finland326948
Academy of Finland310682
Issue or Number:18
DOI:10.5194/acp-21-14275-2021
Record Number:CaltechAUTHORS:20211015-162632786
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20211015-162632786
Official Citation:Xiao, M., Hoyle, C. R., Dada, L., Stolzenburg, D., Kürten, A., Wang, M., Lamkaddam, H., Garmash, O., Mentler, B., Molteni, U., Baccarini, A., Simon, M., He, X.-C., Lehtipalo, K., Ahonen, L. R., Baalbaki, R., Bauer, P. S., Beck, L., Bell, D., Bianchi, F., Brilke, S., Chen, D., Chiu, R., Dias, A., Duplissy, J., Finkenzeller, H., Gordon, H., Hofbauer, V., Kim, C., Koenig, T. K., Lampilahti, J., Lee, C. P., Li, Z., Mai, H., Makhmutov, V., Manninen, H. E., Marten, R., Mathot, S., Mauldin, R. L., Nie, W., Onnela, A., Partoll, E., Petäjä, T., Pfeifer, J., Pospisilova, V., Quéléver, L. L. J., Rissanen, M., Schobesberger, S., Schuchmann, S., Stozhkov, Y., Tauber, C., Tham, Y. J., Tomé, A., Vazquez-Pufleau, M., Wagner, A. C., Wagner, R., Wang, Y., Weitz, L., Wimmer, D., Wu, Y., Yan, C., Ye, P., Ye, Q., Zha, Q., Zhou, X., Amorim, A., Carslaw, K., Curtius, J., Hansel, A., Volkamer, R., Winkler, P. M., Flagan, R. C., Kulmala, M., Worsnop, D. R., Kirkby, J., Donahue, N. M., Baltensperger, U., El Haddad, I., and Dommen, J.: The driving factors of new particle formation and growth in the polluted boundary layer, Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, 2021.
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ID Code:111468
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:18 Oct 2021 17:45
Last Modified:18 Oct 2021 17:45

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