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.
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| 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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| 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. | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| 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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