Iodine oxoacids enhance nucleation of sulfuric acid particles in the atmosphere

Xu-Cheng He; Mario Simon; Siddharth Iyer; Hong-Bin Xie; Birte Rörup; Jiali Shen; Henning Finkenzeller; Dominik Stolzenburg; Rongjie Zhang; Andrea Baccarini; Yee Jun Tham; Mingyi Wang; Stavros Amanatidis; Ana A Piedehierro; Antonio Amorim; Rima Baalbaki; Zoé Brasseur; Lucía Caudillo; Biwu Chu; Lubna Dada; Jonathan Duplissy; Imad El Haddad; Richard C Flagan; Manuel Granzin; Armin Hansel; Martin Heinritzi; Victoria Hofbauer; Tuija Jokinen; Deniz Kemppainen; Weimeng Kong; Jordan Krechmer; Andreas Kürten; Houssni Lamkaddam; Brandon Lopez; Fangfang Ma; Naser G A Mahfouz; Vladimir Makhmutov; Hanna E Manninen; Guillaume Marie; Ruby Marten; Dario Massabò; Roy L Mauldin; Bernhard Mentler; Antti Onnela; Tuukka Petäjä; Joschka Pfeifer; Maxim Philippov; Ananth Ranjithkumar; Matti P Rissanen; Siegfried Schobesberger; Wiebke Scholz; Benjamin Schulze; Mihnea Surdu; Roseline C Thakur; António Tomé; Andrea C Wagner; Dongyu Wang; Yonghong Wang; Stefan K Weber; André Welti; Paul M Winkler; Marcel Zauner-Wieczorek; Urs Baltensperger; Joachim Curtius; Theo Kurtén; Douglas R Worsnop; Rainer Volkamer; Katrianne Lehtipalo; Jasper Kirkby; Neil M Donahue; Mikko Sipilä; Markku Kulmala

doi:10.1126/science.adh2526

Iodine oxoacids enhance nucleation of sulfuric acid particles in the atmosphere

Science. 2023 Dec 15;382(6676):1308-1314. doi: 10.1126/science.adh2526. Epub 2023 Dec 14.

Authors

Xu-Cheng He^{1

2

3}, Mario Simon⁴, Siddharth Iyer⁵, Hong-Bin Xie⁶, Birte Rörup¹, Jiali Shen¹, Henning Finkenzeller^{7

8}, Dominik Stolzenburg^{1

9}, Rongjie Zhang⁶, Andrea Baccarini^{10

11}, Yee Jun Tham^{1

12}, Mingyi Wang¹³, Stavros Amanatidis¹³, Ana A Piedehierro³, Antonio Amorim¹⁴, Rima Baalbaki¹, Zoé Brasseur¹, Lucía Caudillo⁴, Biwu Chu^{1

15}, Lubna Dada^{1

10}, Jonathan Duplissy^{1

16}, Imad El Haddad¹⁰, Richard C Flagan¹³, Manuel Granzin⁴, Armin Hansel¹⁷, Martin Heinritzi⁴, Victoria Hofbauer², Tuija Jokinen^{1

18}, Deniz Kemppainen¹, Weimeng Kong¹³, Jordan Krechmer¹⁹, Andreas Kürten⁴, Houssni Lamkaddam¹⁰, Brandon Lopez^{2

20}, Fangfang Ma⁶, Naser G A Mahfouz², Vladimir Makhmutov^{21

22}, Hanna E Manninen²³, Guillaume Marie⁴, Ruby Marten¹⁰, Dario Massabò²⁴, Roy L Mauldin^{25

26}, Bernhard Mentler¹⁷, Antti Onnela²³, Tuukka Petäjä¹, Joschka Pfeifer²³, Maxim Philippov²¹, Ananth Ranjithkumar²⁷, Matti P Rissanen^{5

28}, Siegfried Schobesberger²⁹, Wiebke Scholz¹⁷, Benjamin Schulze¹³, Mihnea Surdu¹⁰, Roseline C Thakur¹, António Tomé³⁰, Andrea C Wagner⁴, Dongyu Wang¹⁰, Yonghong Wang^{1

15}, Stefan K Weber^{4

23}, André Welti³, Paul M Winkler³¹, Marcel Zauner-Wieczorek⁴, Urs Baltensperger¹⁰, Joachim Curtius⁴, Theo Kurtén²⁸, Douglas R Worsnop^{1

19}, Rainer Volkamer^{7

8}, Katrianne Lehtipalo^{1

3}, Jasper Kirkby^{4

23}, Neil M Donahue^{2

20

25

32}, Mikko Sipilä¹, Markku Kulmala^{1

16

33

34}

Affiliations

¹ Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland.
² Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA.
³ Finnish Meteorological Institute, 00560 Helsinki, Finland.
⁴ Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.
⁵ Aerosol Physics Laboratory, Faculty of Engineering and Natural Sciences, Tampere University, 33720 Tampere, Finland.
⁶ Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, 116024 Dalian, China.
⁷ Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309, USA.
⁸ Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309, USA.
⁹ Institute for Materials Chemistry, TU Wien, 1060 Vienna, Austria.
¹⁰ Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, CH-5232 Villigen, Switzerland.
¹¹ Laboratory of Atmospheric Processes and their Impact, Ecole Polytechnique Fédérale de Lausanne (EPFL), 1015 Lausanne, Switzerland.
¹² School of Marine Sciences, Sun Yat-sen University, 519082 Zhuhai, China.
¹³ Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA.
¹⁴ CENTRA and Faculdade de Ciências da Universidade de Lisboa, 1749-016 Lisboa, Portugal.
¹⁵ Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, 100084 Beijing, China.
¹⁶ Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland.
¹⁷ Institute of Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria.
¹⁸ Climate and Atmosphere Research Centre (CARE-C), The Cyprus Institute, 1645 Nicosia, Cyprus.
¹⁹ Aerodyne Research, Inc., Billerica, MA 01821, USA.
²⁰ Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, PA 15213, USA.
²¹ P. N. Lebedev Physical Institute of the Russian Academy of Sciences, 119991 Moscow, Russia.
²² Moscow Institute of Physics and Technology (National Research University),141701 Moscow, Russian Federation.
²³ CERN, the European Organization for Nuclear Research, CH-1211 Geneva, Switzerland.
²⁴ Department of Physics, University of Genoa, 16146 Genoa, Italy.
²⁵ Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA 15213, USA.
²⁶ Department of Atmospheric and Oceanic Sciences, University of Colorado Boulder, Boulder, CO 80309, USA.
²⁷ Natural Environment Research Council, British Antarctic Survey, CB3 0ET Cambridge, UK.
²⁸ Department of Chemistry, University of Helsinki, 00014 Helsinki, Finland.
²⁹ Department of Applied Physics, University of Eastern Finland, 70211 Kuopio, Finland.
³⁰ Instituto Dom Luiz (IDL)-Universidade da Beira Interior, 6201-001 Covilhã, Portugal.
³¹ Faculty of Physics, University of Vienna, 1090 Wien, Austria.
³² Department of Engineering and Public Policy, Carnegie Mellon University, Pittsburgh, PA 15213, USA.
³³ Joint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, 210023 Nanjing, China.
³⁴ Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, 100029 Beijing, China.

PMID: 38096284
DOI: 10.1126/science.adh2526

Abstract

The main nucleating vapor in the atmosphere is thought to be sulfuric acid (H₂SO₄), stabilized by ammonia (NH₃). However, in marine and polar regions, NH₃ is generally low, and H₂SO₄ is frequently found together with iodine oxoacids [HIO_x, i.e., iodic acid (HIO₃) and iodous acid (HIO₂)]. In experiments performed with the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we investigated the interplay of H₂SO₄ and HIO_x during atmospheric particle nucleation. We found that HIO_x greatly enhances H₂SO₄(-NH₃) nucleation through two different interactions. First, HIO₃ strongly binds with H₂SO₄ in charged clusters so they drive particle nucleation synergistically. Second, HIO₂ substitutes for NH₃, forming strongly bound H₂SO₄-HIO₂ acid-base pairs in molecular clusters. Global observations imply that HIO_x is enhancing H₂SO₄(-NH₃) nucleation rates 10- to 10,000-fold in marine and polar regions.