Synergistic HNO3–H2SO4–NH3 upper tropospheric particle formation

Mingyi Wang, Mao Xiao, Barbara Bertozzi, Guillaume Marie, Birte Rörup, Benjamin Schulze, Roman Bardakov, Xu-Cheng He, Jiali Shen, Wiebke Scholz, Ruby Marten, Lubna Dada, Rima Baalbaki, Brandon Lopez, Houssni Lamkaddam, Hanna E. Manninen, António Amorim, Farnoush Ataei, Pia Bogert, Zoé Brasseur, Lucía Caudillo, Louis-Philippe De Menezes, Jonathan Duplissy, Annica M. L. Ekman, Henning Finkenzeller, Loïc Gonzalez Carracedo, Manuel Granzin, Roberto Guida, Martin Heinritzi, Victoria Hofbauer, Kristina Höhler, Kimmo Korhonen, Jordan E. Krechmer, Andreas Kürten, Katrianne Lehtipalo, Naser G. A. Mahfouz, Vladimir Makhmutov, Dario Massabò, Serge Mathot, Roy L. Mauldin, Bernhard Mentler, Tatjana Müller, Antti Onnela, Tuukka Petäjä, Maxim Philippov, Ana A. Piedehierro, Andrea Pozzer, Ananth Ranjithkumar, Meredith Schervish, Siegfried Schobesberger, Mario Simon, Yuri Stozhkov, António Tomé, Nsikanabasi Silas Umo, Franziska Vogel, Robert Wagner, Dongyu S. Wang, Stefan K. Weber, André Welti, Yusheng Wu, Marcel Zauner-Wieczorek, Mikko Sipilä, Paul M. Winkler, Armin Hansel, Urs Baltensperger, Markku Kulmala, Richard C. Flagan, Joachim Curtius, Ilona Riipinen, Hamish Gordon, Jos Lelieveld, Imad El-Haddad, Rainer Volkamer, Douglas R. Worsnop, Theodoros Christoudias, Jasper Kirkby, Ottmar Möhler and Neil M. Donahue ()
Additional contact information
Mingyi Wang: Carnegie Mellon University
Mao Xiao: Paul Scherrer Institute
Barbara Bertozzi: Karlsruhe Institute of Technology
Guillaume Marie: Goethe University Frankfurt
Birte Rörup: University of Helsinki
Benjamin Schulze: California Institute of Technology
Roman Bardakov: Stockholm University
Xu-Cheng He: University of Helsinki
Jiali Shen: University of Helsinki
Wiebke Scholz: University of Innsbruck
Ruby Marten: Paul Scherrer Institute
Lubna Dada: Paul Scherrer Institute
Rima Baalbaki: University of Helsinki
Brandon Lopez: Carnegie Mellon University
Houssni Lamkaddam: Paul Scherrer Institute
Hanna E. Manninen: CERN, the European Organization for Nuclear Research
António Amorim: CENTRA and Faculdade de Ciências da Universidade de Lisboa
Farnoush Ataei: Leibniz Institute for Tropospheric Research
Pia Bogert: Karlsruhe Institute of Technology
Zoé Brasseur: University of Helsinki
Lucía Caudillo: Goethe University Frankfurt
Louis-Philippe De Menezes: CERN, the European Organization for Nuclear Research
Jonathan Duplissy: University of Helsinki
Annica M. L. Ekman: Stockholm University
Henning Finkenzeller: University of Colorado Boulder
Loïc Gonzalez Carracedo: University of Vienna
Manuel Granzin: Goethe University Frankfurt
Roberto Guida: CERN, the European Organization for Nuclear Research
Martin Heinritzi: Goethe University Frankfurt
Victoria Hofbauer: Carnegie Mellon University
Kristina Höhler: Karlsruhe Institute of Technology
Kimmo Korhonen: University of Eastern Finland
Jordan E. Krechmer: Aerodyne Research, Inc.
Andreas Kürten: Goethe University Frankfurt
Katrianne Lehtipalo: University of Helsinki
Naser G. A. Mahfouz: Carnegie Mellon University
Vladimir Makhmutov: P. N. Lebedev Physical Institute of the Russian Academy of Sciences
Dario Massabò: University of Genoa & INFN
Serge Mathot: CERN, the European Organization for Nuclear Research
Roy L. Mauldin: Carnegie Mellon University
Bernhard Mentler: University of Innsbruck
Tatjana Müller: Goethe University Frankfurt
Antti Onnela: CERN, the European Organization for Nuclear Research
Tuukka Petäjä: University of Helsinki
Maxim Philippov: P. N. Lebedev Physical Institute of the Russian Academy of Sciences
Ana A. Piedehierro: Finnish Meteorological Institute
Andrea Pozzer: Max Planck Institute for Chemistry
Ananth Ranjithkumar: University of Leeds
Meredith Schervish: Carnegie Mellon University
Siegfried Schobesberger: University of Eastern Finland
Mario Simon: Goethe University Frankfurt
Yuri Stozhkov: P. N. Lebedev Physical Institute of the Russian Academy of Sciences
António Tomé: University of Beira Interior
Nsikanabasi Silas Umo: Karlsruhe Institute of Technology
Franziska Vogel: Karlsruhe Institute of Technology
Robert Wagner: Karlsruhe Institute of Technology
Dongyu S. Wang: Paul Scherrer Institute
Stefan K. Weber: CERN, the European Organization for Nuclear Research
André Welti: Finnish Meteorological Institute
Yusheng Wu: University of Helsinki
Marcel Zauner-Wieczorek: Goethe University Frankfurt
Mikko Sipilä: University of Helsinki
Paul M. Winkler: University of Vienna
Armin Hansel: University of Innsbruck
Urs Baltensperger: Paul Scherrer Institute
Markku Kulmala: University of Helsinki
Richard C. Flagan: California Institute of Technology
Joachim Curtius: Goethe University Frankfurt
Ilona Riipinen: Stockholm University
Hamish Gordon: Carnegie Mellon University
Jos Lelieveld: Max Planck Institute for Chemistry
Imad El-Haddad: Paul Scherrer Institute
Rainer Volkamer: University of Colorado Boulder
Douglas R. Worsnop: University of Helsinki
Theodoros Christoudias: The Cyprus Institute
Jasper Kirkby: Goethe University Frankfurt
Ottmar Möhler: Karlsruhe Institute of Technology
Neil M. Donahue: Carnegie Mellon University

Nature, 2022, vol. 605, issue 7910, 483-489

Abstract: Abstract New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)1–4. However, the precursor vapours that drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we show that nitric acid, sulfuric acid and ammonia form particles synergistically, at rates that are orders of magnitude faster than those from any two of the three components. The importance of this mechanism depends on the availability of ammonia, which was previously thought to be efficiently scavenged by cloud droplets during convection. However, surprisingly high concentrations of ammonia and ammonium nitrate have recently been observed in the upper troposphere over the Asian monsoon region5,6. Once particles have formed, co-condensation of ammonia and abundant nitric acid alone is sufficient to drive rapid growth to CCN sizes with only trace sulfate. Moreover, our measurements show that these CCN are also highly efficient ice nucleating particles—comparable to desert dust. Our model simulations confirm that ammonia is efficiently convected aloft during the Asian monsoon, driving rapid, multi-acid HNO3–H2SO4–NH3 nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.

Date: 2022
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DOI: 10.1038/s41586-022-04605-4

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