20 Jan 2021

20 Jan 2021

Review status: this preprint is currently under review for the journal ACP.

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

Mao Xiao1, Christopher R. Hoyle1,2, Lubna Dada3, Dominik Stolzenburg4, Andreas Kürten5, Mingyi Wang6, Houssni Lamkaddam1, Olga Garmash3, Bernhard Mentler7, Ugo Molteni1, Andrea Baccarini1, Mario Simon5, Xu-Cheng He3, Katrianne Lehtipalo3,8, Lauri R. Ahonen3, Rima Baalbaki3, Paulus S. Bauer4, Lisa Beck3, David Bell1, Federico Bianchi3, Sophia Brilke4, Dexian Chen6, Randall Chiu9, António Dias10, Jonathan Duplissy3,11, Henning Finkenzeller9, Hamish Gordon12, Victoria Hofbauer6, Changhyuk Kim13,14, Theodore K. Koenig9, Janne Lampilahti3, Chuan Ping Lee1, Zijun Li15, Huajun Mai13, Vladimir Makhmutov16, Hanna E. Manninen17, Ruby Marten1, Serge Mathot17, Roy L. Mauldin18,19, Wei Nie20, Antti Onnela17, Eva Partoll7, Tuukka Petäjä3, Joschka Pfeifer5,17, Veronika Pospisilova1, Lauriane L. J. Quéléver3, Matti Rissanen3,a, Siegfried Schobesberger15, Simone Schuchmann17, Yuri Stozhkov16, Christian Tauber4, Yee Jun Tham3, António Tomé21, Miguel Vazquez-Pufleau4, Andrea C. Wagner5,9,b, Robert Wanger3, Yonghong Wang3, Lena Weitz5, Daniela Wimmer3,4, Yusheng Wu3, Chao Yan3, Penglin Ye6,22, Qing Ye6, Qiaozhi Zha3, Xueqin Zhou5, Antonio Amorim10, Ken Carslaw12, Joachim Curtius5, Armin Hansel7, Rainer Volkamer9,19, Paul M. Winkler4, Richard C. Flagan13, Markku Kulmala3,11,20,23, Douglas R. Worsnop3,22, Jasper Kirkby5,17, Neil M. Donahue6, Urs Baltensperger1, Imad El Haddad1, and Josef Dommen1 Mao Xiao et al.
  • 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
  • 2Institute for Atmospheric and Climate Science, ETH Zurich, 8092 Zurich, Switzerland
  • 3Institute for Atmospheric and Earth System Research (INAR) / Physics, University of Helsinki, 00014 Helsinki, Finland
  • 4Faculty of Physics, University of Vienna, 1090 Vienna, Austria
  • 5Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
  • 6Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA
  • 7Institute of Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
  • 8Finnish Meteorological Institute, 00560 Helsinki, Finland
  • 9Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO 80305, USA
  • 10CENTRA and FCUL, University of Lisbon, 1749-016 Lisbon, Portugal
  • 11Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland
  • 12University of Leeds, LS2 9JT Leeds, United Kingdom
  • 13Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA
  • 14School of Civil and Environmental Engineering, Pusan National University, 46241 Busan, Republic of Korea
  • 15Department of Applied Physics, University of Eastern Finland, 70211 Kuopio, Finland
  • 16P.N. Lebedev Physical Institute of the Russian Academy of Sciences, 119991 Moscow, Russian Federation
  • 17CERN, CH-1211, Geneva, Switzerland
  • 18Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA 15213, USA
  • 19Department of Oceanic and Atmospheric Sciences, University of Colorado Boulder, Boulder, CO 80309, USA
  • 20Joint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, Nanjing, Jiangsu Province, China
  • 21IDL-Universidade da Beira Interior, Covilhã, Portugal
  • 22Aerodyne Research Inc., Billerica, MA 01821-3976, USA
  • 23Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China
  • anow at: Aerosol Physics Laboratory, Physics Unit, Faculty of Engineering and Natural Sciences, Tampere University, Tampere, Finland
  • bnow at: Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO 80305, USA

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 four orders of magnitude and the reasons behind this variability 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 are 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.

Mao Xiao et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2020-1323', Anonymous Referee #1, 19 Feb 2021
  • RC2: 'Comment on acp-2020-1323', Anonymous Referee #2, 19 Mar 2021

Mao Xiao et al.


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Short summary
Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid-base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span the four orders of magnitude variation of observed NPF rates in the ambient. We provide a framework based on NPF and growth rates to interpret ambient observations.