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

Mauldin, Roy L; Koenig, Theodore K; Chiu, Randall; Finkenzeller, Henning

Citeable URL: https://scholar.colorado.edu/concern/articles/w66345088

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.

Full List of Authors:

Mao Xiao¹, Christopher R. Hoyle^1,2, Lubna Dada³, Dominik Stolzenburg⁴, Andreas Kürten⁵, Mingyi Wang⁶, Houssni Lamkaddam¹, Olga Garmash³, Bernhard Mentler⁷, Ugo Molteni¹, Andrea Baccarini¹, Mario Simon⁵, Xu-Cheng He³, Katrianne Lehtipalo^3,8, Lauri R. Ahonen³, Rima Baalbaki³, Paulus S. Bauer⁴, Lisa Beck³, David Bell¹, Federico Bianchi³, Sophia Brilke⁴, Dexian Chen⁶, Randall Chiu⁹, António Dias¹⁰, Jonathan Duplissy^3,11, Henning Finkenzeller⁹, Hamish Gordon⁶, Victoria Hofbauer⁶, Changhyuk Kim^13,14, Theodore K. Koenig^9,a, Janne Lampilahti³, Chuan Ping Lee¹, Zijun Li¹⁵, Huajun Mai¹³, Vladimir Makhmutov¹⁶, Hanna E. Manninen¹⁷, Ruby Marten¹, Serge Mathot¹⁷, Roy L. Mauldin^18,19, Wei Nie²⁰, Antti Onnela¹⁷, Eva Partoll⁷, Tuukka Petäjä³, Joschka Pfeifer^5,17, Veronika Pospisilova¹, Lauriane L. J. Quéléver³, Matti Rissanen^3,b, Siegfried Schobesberger¹⁵, Simone Schuchmann^17,c, Yuri Stozhkov¹⁶, Christian Tauber⁴, Yee Jun Tham³, António Tomé²¹, Miguel Vazquez-Pufleau⁴, Andrea C. Wagner^5,9,d, Robert Wagner³, Yonghong Wang³, Lena Weitz⁵, Daniela Wimmer^3,4, Yusheng Wu³, Chao Yan³, Penglin Ye^6,22, Qing Ye⁶, Qiaozhi Zha³, Xueqin Zhou⁵, Antonio Amorim¹⁰, Ken Carslaw¹², Joachim Curtius⁵, Armin Hansel⁷, Rainer Volkamer^9,19, Paul M. Winkler⁴, Richard C. Flagan¹³, Markku Kulmala^3,11,20,23, Douglas R. Worsnop^3,22, Jasper Kirkby^5,17, Neil M. Donahue⁶, Urs Baltensperger¹, Imad El Haddad¹, and Josef Dommen¹
- 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
- ⁸Atmospheric Composition Research Unit, Finnish Meteorological Institute, 00560 Helsinki, Finland
- ⁹Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO 80309, USA
- ¹⁰CENTRA and FCUL, University of Lisbon, 1749-016 Lisbon, Portugal
- ¹¹Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland
- ¹²School of Earth and Environment, University 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
- ¹⁶Solar and Cosmic Ray Physics Laboratory, P.N. Lebedev Physical Institute of the Russian Academy of Sciences, 119991 Moscow, Russian Federation
- ¹⁷CERN, 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: College of Environmental Sciences and Engineering, Peking University, 100871 Beijing, China
- ^bnow at: Aerosol Physics Laboratory, Physics Unit, Faculty of Engineering and Natural Sciences, Tampere University, 33720 Tampere, Finland
- ^cnow at: Experimentelle Teilchen- und Astroteilchenphysik, Johannes Gutenberg University Mainz, 55128 Mainz, Germany
- ^dnow at: Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO 80305, USA
Correspondence: Urs Baltensperger (urs.baltensperger@psi.ch) and Imad El Haddad (imad.el-haddad@psi.ch)

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