CaltechAUTHORS
  A Caltech Library Service

Rapid growth of new atmospheric particles by nitric acid and ammonia condensation

Wang, Mingyi and Kong, Weimeng and Marten, Ruby and He, Xu-Cheng and Chen, Dexian and Pfeifer, Joschka and Heitto, Arto and Kontkanen, Jenni and Dada, Lubna and Kürten, Andreas and Yli-Juuti, Taina and Manninen, Hanna E. and Amanatidis, Stavros and Amorim, Antonio and Baalbaki, Rima and Baccarini, Andrea and Bell, David M. and Bertozzi, Barbara and Bräkling, Steffen and Brilke, Sophia and Murillo, Lucía Caudillo and Chiu, Randall and Chu, Biwu and De Menezes, Louis-Philippe and Duplissy, Jonathan and Finkenzeller, Henning and Carracedo, Loic Gonzalez and Granzin, Manuel and Guida, Roberto and Hansel, Armin and Hofbauer, Victoria and Krechmer, Jordan and Lehtipalo, Katrianne and Lamkaddam, Houssni and Lampimäki, Markus and Lee, Chuan Ping and Makhmutov, Vladimir and Marie, Guillaume and Mathot, Serge and Mauldin, Roy L. and Mentler, Bernhard and Müller, Tatjana and Onnela, Antti and Partoll, Eva and Petäjä, Tuukka and Philippov, Maxim and Pospisilova, Veronika and Ranjithkumar, Ananth and Rissanen, Matti and Rörup, Birte and Scholz, Wiebke and Shen, Jiali and Simon, Mario and Sipilä, Mikko and Steiner, Gerhard and Stolzenburg, Dominik and Tham, Yee Jun and Tomé, António and Wagner, Andrea C. and Wang, Dongyu S. and Wang, Yonghong and Weber, Stefan K. and Winkler, Paul M. and Wlasits, Peter J. and Wu, Yusheng and Xiao, Mao and Ye, Qing and Zauner-Wieczorek, Marcel and Zhou, Xueqin and Volkamer, Rainer and Riipinen, Ilona and Dommen, Josef and Curtius, Joachim and Baltensperger, Urs and Kulmala, Markku and Worsnop, Douglas R. and Kirkby, Jasper and Seinfeld, John H. and El-Haddad, Imad and Flagan, Richard C. and Donahue, Neil M. (2020) Rapid growth of new atmospheric particles by nitric acid and ammonia condensation. Nature, 581 (7807). pp. 184-189. ISSN 0028-0836. https://resolver.caltech.edu/CaltechAUTHORS:20200313-092203655

[img] PDF - Published Version
Creative Commons Attribution.

2706Kb
[img] Image (JPEG) (Extended Data Fig. 1: New-particle-formation events observed in various remote and urban environments (see Extended Data Table 3 for a complete set of references)) - Supplemental Material
Creative Commons Attribution.

80Kb
[img] Image (JPEG) (Extended Data Fig. 2: Activation diameter of newly formed particles) - Supplemental Material
Creative Commons Attribution.

177Kb
[img] Image (JPEG) (Extended Data Fig. 3: A typical measurement sequence) - Supplemental Material
Creative Commons Attribution.

128Kb
[img] Image (JPEG) (Extended Data Fig. 4: Comparison of growth rates and chemical composition in four simulations at +5 °C and −10 °C with the thermodynamic model MABNAG) - Supplemental Material
Creative Commons Attribution.

172Kb
[img] Image (JPEG) (Extended Data Fig. 5: Combined particle-size distribution and total concentrations from four particle characterization instruments) - Supplemental Material
Creative Commons Attribution.

91Kb
[img] Image (JPEG) (Extended Data Fig. 6: Determination of growth rate using the appearance-time method) - Supplemental Material
Creative Commons Attribution.

112Kb
[img] Image (JPEG) (Extended Data Fig. 7: Saturation ratio as a function of temperature) - Supplemental Material
Creative Commons Attribution.

70Kb
[img] MS Excel (Source Data Fig. 1) - Supplemental Material
Creative Commons Attribution.

65Kb
[img] MS Excel (Source Data Fig. 2) - Supplemental Material
Creative Commons Attribution.

128Kb
[img] MS Excel (Source Data Fig. 3) - Supplemental Material
Creative Commons Attribution.

13Kb
[img] MS Excel (Source Data Fig. 4) - Supplemental Material
Creative Commons Attribution.

2425Kb
[img] MS Excel (Source Data Extended Data Fig. 1) - Supplemental Material
Creative Commons Attribution.

54Kb
[img] MS Excel (Source Data Extended Data Fig. 2) - Supplemental Material
Creative Commons Attribution.

47Kb
[img] MS Excel (Source Data Extended Data Fig. 3) - Supplemental Material
Creative Commons Attribution.

24Kb
[img] MS Excel (Source Data Extended Data Fig. 4) - Supplemental Material
Creative Commons Attribution.

9Kb
[img] MS Excel (Source Data Extended Data Fig. 5) - Supplemental Material
Creative Commons Attribution.

39Kb
[img] MS Excel (Source Data Extended Data Fig. 6) - Supplemental Material
Creative Commons Attribution.

5Mb
[img] MS Excel (Source Data Extended Data Fig. 7) - Supplemental Material
Creative Commons Attribution.

13Kb

Use this Persistent URL to link to this item: https://resolver.caltech.edu/CaltechAUTHORS:20200313-092203655

Abstract

A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog, but how it occurs in cities is often puzzling. If the growth rates of urban particles are similar to those found in cleaner environments (1–10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below −15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid–base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1038/s41586-020-2270-4DOIArticle
https://doi.org/10.5281/zenodo.3653377DOIData
https://pubs.acs.org/doi/10.1021/cen-09819-scicon1Featured InC&EN - Science Concentrates
ORCID:
AuthorORCID
Wang, Mingyi0000-0001-5782-2513
Kong, Weimeng0000-0002-9432-2857
Amanatidis, Stavros0000-0002-4924-8424
Seinfeld, John H.0000-0003-1344-4068
Flagan, Richard C.0000-0001-5690-770X
Additional Information:© 2020 Springer Nature Limited. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. Received 26 September 2019; Accepted 17 March 2020; Published 13 May 2020. We thank the European Organization for Nuclear Research (CERN) for supporting CLOUD with technical and financial resources and for providing a particle beam from the CERN Proton Synchrotron. This research has received funding from the US National Science Foundation (NSF; grant numbers AGS1602086, AGS1801329 and AGS-1801280); a NASA graduate fellowship (grant number NASA-NNX16AP36H); a Carnegie Mellon University Scott Institute Visiting Fellows grant; the Swiss National Science Foundation (grant numbers 200021_169090, 200020_172602 and 20FI20_172622); the European Community (EC) Seventh Framework Programme and the European Union (EU) H2020 programme (Marie Skłodowska Curie ITN CLOUD-TRAIN grant number 316662 and CLOUD-MOTION grant number 764991); a European Research Council (ERC) Advanced Grant (number ATM-GP 227463); an ERC Consolidator Grant (NANODYNAMITE 616075); an ERC Starting Grant (GASPARCON 714621), the Academy of Finland (grants 306853, 296628, 316114 and 299544); the Academy of Finland Center of Excellence programme (grant 307331); the German Federal Ministry of Education and Research (CLOUD-12 number 01LK1222A and CLOUD-16 number 01LK1601A); the Knut and Alice Wallenberg Foundation Wallenberg Academy Fellow project AtmoRemove (grant number 2015.0162); the Austrian Science Fund (grant number P 27295-N20); the Portuguese Foundation for Science and Technology (grant number CERN/FIS-COM/0014/2017); and the Presidium of the Russian Academy of Sciences (‘High energy physics and neutrino astrophysics’ 2015). The FIGAERO-CIMS was supported by a Major Research Instrumentation (MRI) grant for the US NSF (AGS-1531284), and by the Wallace Research Foundation. We thank H. Cawley for producing Fig. 4a. Data availability: The full dataset shown in the figures and tables is publicly available(58). All data shown in the figures and tables and additional raw data are available upon request from the corresponding author. Source data for Figs. 1–4 and Extended Data Figs. 1–7 are provided with the paper. Code availability: Codes for the MABNAG and nano-Köhler simulations and for conducting the analysis presented here can be obtained upon request from the corresponding author. Author Contributions: M.W., R.M., J. Dommen, U.B., J. Kirkby, I.E-H. and N.M.D. planned the experiments. M.W., W.K., R.M., X-C.H., D.C., J.P., A.K., H.E.M., S.A., A.B., S. Bräkling, S. Brilke, L.C.M., B.C., L-P.D.M., J. Duplissy, H.F., L.G.C., M.G., R.G., A. Hansel, V.H., J.K., K.L., H.L., C.P.L., V.M., G.M., S.M., B.M., T.M., A.O., E.P., T.P., M.P., V.P., M.R., B.R., W.S., J.S., M. Simon, M. Sipilä, G.S., D.S., Y.J.T., A.T., R.V., A.C.W., D.S.W., Y. Wang, S.K.W., P.M.W., P.J.W., Y. Wu, Q.Y., M.Z.-W., X.Z., J. Kirkby, I.E.-H. and R.C.F. prepared the CLOUD facility or measuring instruments. M.W., W.K., R.M., X.-C.H., D.C., J.P., L.D., H.E.M., S.A., A.A., R.B., A.B., D.M.B., B.B., S. Bräkling, S. Brilke, R.C., H.F., L.G.C., M.G., V.H., J.S., J. Duplissy, H.L., M.L., C.P.L., V.M., G.M., R.L.M., B.M., T.M., E.P., V.P., A.R., M.R., B.R., W.S., M. Simon, G.S., D.S., Y.J.T., A.T., A.C.W., D.S.W., Y. Wang, S.K.W., P.M.W., P.J.W., Y. Wu, M.X., M.Z.-W., X.Z., J. Kirkby and I.E.-H. collected the data. M.W., W.K., R.M., X.-C.H., D.C., J.P., A. Heitto, J. Kontkanen, L.D., A.K., T.Y.-J., H.E.M., S.A., L.G.C., J.S., W.S., M. Simon, D.S., D.S.W., S.K.W., P.M.W., I.E.-H., R.C.F. and N.M.D. analysed the data. M.W., W.K., R.M., X.-C.H., D.C., A. Heitto, J. Kontkanen, T.Y.-J., H.E.M., D.M.B., H.L., D.S., R.V., M.X., I.R., J. Dommen, J.C., U.B., M.K., D.R.W., J. Kirkby, J.H.S., I.E.-H., R.C.F. and N.M.D. contributed to the scientific discussion. M.W., W.K., R.M., X.-C.H., D.C., J.P., A. Heitto, J. Kontkanen, T.Y.-J., I.R., J. Dommen, U.B., M.K., D.R.W., J. Kirkby, J.H.S., I.E.-H., R.C.F. and N.M.D. wrote the manuscript. The authors declare no competing interests. Peer review information: Nature thanks Hugh Coe and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Funders:
Funding AgencyGrant Number
CERNUNSPECIFIED
NSFAGS-1602086
NSFAGS-1801329
NSFAGS-1801280
NASANNX16AP36
Carnegie Mellon UniversityUNSPECIFIED
Swiss National Science Foundation (SNSF)200021_169090
Swiss National Science Foundation (SNSF)200020_172602
Swiss National Science Foundation (SNSF)20FI20_172622
Marie Curie Fellowship316662
Marie Curie Fellowship764991
European Research Council (ERC)227463
European Research Council (ERC)616075
European Research Council (ERC)714621
Academy of Finland306853
Academy of Finland296628
Academy of Finland316114
Academy of Finland299544
Academy of Finland307331
Bundesministerium für Bildung und Forschung (BMBF)01LK1222A
Bundesministerium für Bildung und Forschung (BMBF)01LK1601A
Knut and Alice Wallenberg Foundation2015.0162
Fonds zur Förderung der wissenschaftlichen Forschung (FWF)P 27295-N20
Fundação para a Ciência e a Tecnologia (FCT)CERN/FIS-COM/0014/2017
Russian Academy of SciencesUNSPECIFIED
NSFAGS-1531284
Wallace Coulter FoundationUNSPECIFIED
Subject Keywords:Atmospheric science; Climate change
Issue or Number:7807
Record Number:CaltechAUTHORS:20200313-092203655
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200313-092203655
Official Citation:Wang, M., Kong, W., Marten, R. et al. Rapid growth of new atmospheric particles by nitric acid and ammonia condensation. Nature 581, 184–189 (2020). https://doi.org/10.1038/s41586-020-2270-4
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:101901
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:27 Apr 2020 18:31
Last Modified:18 May 2020 20:02

Repository Staff Only: item control page