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Discussion papers
https://doi.org/10.5194/acp-2019-755
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-755
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 15 Nov 2019

Submitted as: research article | 15 Nov 2019

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Enhanced growth rate of atmospheric particles from sulfuric acid

Dominik Stolzenburg1, Mario Simon2, Ananth Ranjithkumar3, Andreas Kürten2, Katrianne Lehtipalo4,5, Hamish Gordon3, Tuomo Nieminen4, Lukas Pichelstorfer4, Xu-Cheng He4, Sophia Brilke1, Mao Xiao6, António Amorim7, Rima Baalbaki4, Andrea Baccarini6, Lisa Beck4, Steffen Bräkling8, Lucía Caudillo Murillo2, Dexian Chen9, Biwu Chu4, Lubna Dada4, António Dias7, Josef Dommen6, Jonathan Duplissy4, Imad El Haddad6, Henning Finkenzeller10, Lukas Fischer11, Loic Gonzalez Carracedo1, Martin Heinritzi2, Changhyuk Kim12,13, Theodore K. Koenig10, Weimeng Kong12, Houssni Lamkaddam6, Chuan Ping Lee6, Markus Leiminger11,14, Zijun Li15, Vladimir Makhmutov16, Hanna E. Manninen17, Guillaume Marie2, Ruby Marten6, Tatjana Müller2, Wei Nie18, Eva Partoll11, Tuukka Petäjä4, Joschka Pfeifer17, Maxim Philippov16, Matti P. Rissanen4,19, Birte Rörup4, Siegfried Schobesberger15, Simone Schuchmann17, Jiali Shen4, Mikko Sipilä4, Gerhard Steiner11, Yuri Stozhkov16, Christian Tauber1, Yee Jun Tham4, António Tomé20, Miguel Vazquez-Pufleau1, Andrea C. Wagner2,10, Mingyi Wang9, Yonghong Wang4, Stefan K. Weber17, Daniela Wimmer1,4, Peter J. Wlasits1, Yusheng Wu4, Qing Ye9, Marcel Zauner-Wieczorek2, Urs Baltensperger6, Kenneth S. Carslaw3, Joachim Curtius2, Neil M. Donahue9, Richard C. Flagan12, Armin Hansel11,14, Markku Kulmala4, Rainer Volkamer10, Jasper Kirkby2,17, and Paul M. Winkler1 Dominik Stolzenburg et al.
  • 1Faculty of Physics, University of Vienna, 1090 Vienna, Austria
  • 2Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
  • 3School of Earth and Environment, University of Leeds, Leeds LS2 9JT, UK
  • 4Institute forAtmospheric and Earth System Research/Physics, University of Helsinki, 00014 Helsinki, Finland
  • 5Finnish Meteorological Institute, 00560 Helsinki, Finland
  • 6Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
  • 7Center for Astrophysics and Gravitation, Faculty of Sciences of the University of Lisbon, 1749-016 Lisbon, Portugal
  • 8Tofwerk AG, 3600 Thun, Switzerland
  • 9Center for Atmospheric Particle Studies, Carnegie Mellon University, 15217 Pittsburgh PA, USA
  • 10Department of Chemistry and Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, 80309 Boulder CO, USA
  • 11Institute for Ion Physics and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
  • 12Division of Chemistryand Chemical Engineering, California Institute of Technology, 91125 Pasadena CA, USA
  • 13Department of Environmental Engineering, Pusan National University, Busan 46241, Republic of Korea
  • 14Ionicon Analytik GmbH, 6020 Innsbruck, Austria
  • 15Department of Applied Physics, University of Eastern Finland, 70211 Kuopio, Finland
  • 16P.N. Lebedev Physical Institute of the Russian Academy of Sciences, 119991 Moscow, Russia
  • 17CERN, the European Organization for Nuclear Research, 1211 Geneva, Switzerland
  • 18Joint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, 210023 Nanjing, China
  • 19Aerosol Physics Laboratory, Tampere University, 33101 Tampere, Finland
  • 20Institute Infante Dom Luíz, University of Beira Interior, 6200-001 Covilhã, Portugal

Abstract. In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles (< 10 nm) from sulfuric acid vapour remain poorly measured. Therefore, the effect of stabilizing bases, the contribution of ions and the impact of attractive forces on molecular collisions are under debate. Here we present precise growth-rate measurements of uncharged sulfuric acid particles in the size range 1.8–10 nm, performed under atmospheric conditions in the CERN CLOUD chamber. Our results show that the evaporation of sulfuric acid particles above 2 nm is indeed negligible and growth proceeds kinetically even at low ammonia concentrations. The experimental growth rates exceed the geometric hard-sphere kinetic limit for condensation of sulfuric acid, and reveal an enhancement resulting from dipole-induced dipole interactions between the vapour molecules and particles. We are able to disentangle the effect of charge-dipole interactions and van-der-Waals forces and observe a steep increase of particle growth rates with decreasing size. Including the experimental results in a global model, we find the enhanced growth rate of sulfuric acid particles increases predicted particle number concentrations in the upper free troposphere by more than 50 %.

Dominik Stolzenburg et al.
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Short summary
Sulfuric acid is a major atmospheric vapour for aerosol formation. If the new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory setup, we demonstrate that van-der-Waals forces enhance particle growth from sulfuric acid. We show in a climate model that this impacts the global aerosol budget. We disentangle the influence of ammonia and ions presenting the first complete picture for sulfuric acid growth from molecular clusters onwards.
Sulfuric acid is a major atmospheric vapour for aerosol formation. If the new particles grow...
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