Widespread detection of chlorine oxyacids in the Arctic atmosphere

Yee Jun Tham (), Nina Sarnela, Siddharth Iyer, Qinyi Li, Hélène Angot, Lauriane L. J. Quéléver, Ivo Beck, Tiia Laurila, Lisa J. Beck, Matthew Boyer, Javier Carmona-García, Ana Borrego-Sánchez, Daniel Roca-Sanjuán, Otso Peräkylä, Roseline C. Thakur, Xu-Cheng He, Qiaozhi Zha, Dean Howard, Byron Blomquist, Stephen D. Archer, Ludovic Bariteau, Kevin Posman, Jacques Hueber, Detlev Helmig, Hans-Werner Jacobi, Heikki Junninen, Markku Kulmala, Anoop S. Mahajan, Andreas Massling, Henrik Skov, Mikko Sipilä, Joseph S. Francisco, Julia Schmale, Tuija Jokinen () and Alfonso Saiz-Lopez ()
Additional contact information
Yee Jun Tham: University of Helsinki
Nina Sarnela: University of Helsinki
Siddharth Iyer: Tampere University
Qinyi Li: Institute of Physical Chemistry Rocasolano, CSIC
Hélène Angot: École Polytechnique Fédérale de Lausanne, (EPFL) Valais Wallis
Lauriane L. J. Quéléver: University of Helsinki
Ivo Beck: École Polytechnique Fédérale de Lausanne, (EPFL) Valais Wallis
Tiia Laurila: University of Helsinki
Lisa J. Beck: University of Helsinki
Matthew Boyer: University of Helsinki
Javier Carmona-García: Universitat de València
Ana Borrego-Sánchez: CSIC-University of Granada
Daniel Roca-Sanjuán: Universitat de València
Otso Peräkylä: University of Helsinki
Roseline C. Thakur: University of Helsinki
Xu-Cheng He: University of Helsinki
Qiaozhi Zha: University of Helsinki
Dean Howard: University of Colorado
Byron Blomquist: University of Colorado
Stephen D. Archer: Bigelow Laboratory for Ocean Sciences, East Boothbay
Ludovic Bariteau: University of Colorado
Kevin Posman: Bigelow Laboratory for Ocean Sciences, East Boothbay
Jacques Hueber: University of Colorado
Detlev Helmig: University of Colorado
Hans-Werner Jacobi: Univ. Grenoble Alpes, CNRS, INRAE, IRD, Grenoble INP, IGE
Heikki Junninen: University of Tartu
Markku Kulmala: University of Helsinki
Anoop S. Mahajan: Ministry of Earth Sciences
Andreas Massling: iClimate, Aarhus University
Henrik Skov: iClimate, Aarhus University
Mikko Sipilä: University of Helsinki
Joseph S. Francisco: University of Pennsylvania
Julia Schmale: École Polytechnique Fédérale de Lausanne, (EPFL) Valais Wallis
Tuija Jokinen: University of Helsinki
Alfonso Saiz-Lopez: Institute of Physical Chemistry Rocasolano, CSIC

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Chlorine radicals are strong atmospheric oxidants known to play an important role in the depletion of surface ozone and the degradation of methane in the Arctic troposphere. Initial oxidation processes of chlorine produce chlorine oxides, and it has been speculated that the final oxidation steps lead to the formation of chloric (HClO3) and perchloric (HClO4) acids, although these two species have not been detected in the atmosphere. Here, we present atmospheric observations of gas-phase HClO3 and HClO4. Significant levels of HClO3 were observed during springtime at Greenland (Villum Research Station), Ny-Ålesund research station and over the central Arctic Ocean, on-board research vessel Polarstern during the Multidisciplinary drifting Observatory for the Study of the Arctic Climate (MOSAiC) campaign, with estimated concentrations up to 7 × 106 molecule cm−3. The increase in HClO3, concomitantly with that in HClO4, was linked to the increase in bromine levels. These observations indicated that bromine chemistry enhances the formation of OClO, which is subsequently oxidized into HClO3 and HClO4 by hydroxyl radicals. HClO3 and HClO4 are not photoactive and therefore their loss through heterogeneous uptake on aerosol and snow surfaces can function as a previously missing atmospheric sink for reactive chlorine, thereby reducing the chlorine-driven oxidation capacity in the Arctic boundary layer. Our study reveals additional chlorine species in the atmosphere, providing further insights into atmospheric chlorine cycling in the polar environment.

Date: 2023
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DOI: 10.1038/s41467-023-37387-y

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