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Attribution of ground-level ozone to anthropogenic and natural sources of NO x and reactive carbon in a global chemical transport model

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Butler, Tim, Lupascu, Aurelia, Nalam, Aditya·2020·Atmospheric chemistry and physics

DOI 10.5194/acp-2020-436

Preprint — published as 10.5194/acp-20-10707-2020

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Abstract

Abstract. We perform a source attribution for tropospheric and ground-level ozone using a novel technique which accounts separately for the contributions of the two chemically distinct emitted precursors (reactive carbon and oxides of nitrogen) to the chemical production of ozone in the troposphere. By tagging anthropogenic emissions of these precursors according to the geographical region from which they are emitted, we determine source/receptor relationships for ground-level ozone. Our methodology reproduces earlier results obtained through other techniques for ozone source attribution, and also delivers additional information about the modelled processes responsible for intercontinental transport of ozone, which is especially strong during the spring months. The current generation of chemical transport models used to support international negotiations aimed at reducing the intercontinental transport of ozone show especially strong inter-model differences in simulated springtime ozone. Current models also simulate a large range of different responses of surface ozone to methane, one of the major precursors of ground-level ozone. Using our novel source attribution technique, we show that emissions of NOx from international shipping over the high seas play a disproportionately strong role in our model system to the hemispheric-scale response of surface ozone to changes in methane, as well as to the springtime maximum in intercontinental transport of ozone and its precursors. We recommend a renewed focus on improvement of the representation of the chemistry of ship NOx emissions in current-generation models. We demonstrate the utility of ozone source attribution as a powerful model diagnostic tool, and recommend that similar source attribution techniques become a standard part of future model inter-comparison studies.

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Authors: Butler, T., Lupascu, A., & Nalam, A.
Affiliations: Research Institute for Sustainability at GFZ (DE)
Corresponding author: Butler, Tim
ORCID: Butler, Tim
Lupascu, Aurelia
Nalam, Aditya
Venue: Atmospheric chemistry and physics
Publisher: Copernicus GmbH
Published: 2020-05-20
Volume: 20
Issue: 17
Pages: 10707-10731
ISSN: 1680-7316 (ISSN-L)
DOI: 10.5194/acp-2020-436
OpenAlex: W3028207660
Cited by: 101
References: 80
Citations by year: 2026: 12 · 2025: 17 · 2024: 27 · 2023: 20 · 2022: 19 · 2021: 6
FWCI: 3.69
Type: journal article
Language: en
Open access: gold
doi.org
Licence: cc-by
creativecommons.org/licenses/by/4.0/ (vor)
Locations: Atmospheric chemistry and physics (publishedVersion, cc-by)
Refubium (Universitätsbibliothek der Freien Universität Berlin) (submittedVersion, cc-by)
DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Publication Database IASS (Institute for Advanced Sustainability Studies (IASS)) (submittedVersion, other-oa)
Universitätsbibliothek der FU Berlin Hochschulschriftenstelle u. Dokumentenserver (cc-by)
Funders: Bundesministerium für Bildung und Forschung
Brandenburger Staatsministerium für Wissenschaft, Forschung und Kultur
Topics: Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric chemistry and aerosols
Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric Ozone and Climate
Physical Sciences › Environmental Science › Global and Planetary Change › Atmospheric and Environmental Gas Dynamics
Keywords: surface ozone, nitrogen oxides, reactive carbon, source-receptor relationships, ship emissions, methane, tropospheric chemistry

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Attribution of ground-level ozone to anthropogenic and natural sources of NO x and reactive carbon in a global chemical transport model

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