Published October 27, 2025
| Version v1
Journal article
Global impact of anthropogenic NH3 emissions on upper tropospheric aerosol formation
Creators
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Xenofontos, Christos1
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Kohl, Matthias2
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Ruhl, Samuel2
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Almeida, João3
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Caudillo-Plath, Lucía4
- Cruz-Simbron, Romulo5
- Dada, Lubna6
- Duplissy, Jonathan7
- Ehrhart, Sebastian2
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Finkenzeller, Henning7
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Höhler, Kristina8
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Kong, Weimeng9
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Kunkler, Felix2
- Lietzke, Clara J.5
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Mentler, Bernhard10
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Morawiec, Aleksandra11
- Onnela, Antti3
- Rato, Pedro3
- Rörup, Birte7
- Russell, Douglas M.4
- Wang, Mingyi12
- 1. The Cyprus Institute
- 2. Max Planck Institute for Chemistry
- 3. The European Organization for Nuclear Research
- 4. Goethe University Frankfurt
- 5. University of Colorado Boulder
- 6. Paul Scherrer Institute
- 7. University of Helsinki
- 8. Karlsruhe Institute of Technology
- 9. California Institute of Technology
- 10. University of Innsbruck
- 11. University of Vienna
- 12. University of Chicago
Description
Anthropogenic ammonia (NH 3 ) emissions have significantly increased in recent decades due to enhanced agricultural activities, contributing to global air pollution. While the effects of NH 3 on surface air quality are well documented, its influence on particle dynamics in the upper troposphere-lower stratosphere (UTLS) and related aerosol impacts remain unquantified. NH 3 reaches the UTLS through convective transport and can enhance new particle formation (NPF). This modeling study evaluates the global impact of anthropogenic NH 3 on UTLS particle formation and quantifies its effects on aerosol loading and cloud condensation nuclei (CCN) abundance. We use the EMAC Earth system model, incorporating multicomponent NPF parameterizations from the CERN CLOUD experiment. Our simulations reveal that convective transport increases NH 3 -driven NPF in the UTLS by one to three orders of magnitude compared to a baseline scenario without anthropogenic NH 3 , causing a doubling of aerosol numbers over high-emission regions. These aerosol changes induce a 2.5-fold increase in upper tropospheric CCN concentrations. Anthropogenic NH 3 emissions increase the relative contribution of water-soluble inorganic ions to the UTLS aerosol optical depth (AOD) by 20% and increase total column AOD by up to 80%. In simulations without anthropogenic NH 3 , UTLS aerosol composition is dominated by sulfate and organic species, with a marked reduction in ammonium nitrate and aerosol water content. This results in a decline of aerosol mass concentration by up to 50%. These findings underscore the profound global influence of anthropogenic NH 3 emissions on UTLS particle formation, AOD, and CCN production, with important implications for cloud formation and climate.
Data availability
The EMAC (ECHAM/MESSy Atmospheric Chemistry) model is continuously developed and used by a consortium of institutions. Members of institutions within the MESSy consortium are granted a license to use MESSy and access its source code. Institutions can join the consortium by signing the MESSy Memorandum of Understanding. Further information is available on the MESSy consortium website (https://www.messy-interface.org) (98). The results presented in this paper were produced using MESSy version 2.55.2. A permanent identifier (DOI: https://doi.org/10.5281/zenodo.14875637) (99) has been assigned in Zenodo under the "CERN CLOUD experiment community." This includes the EMAC configuration files, namelist setup, chemical mechanisms, and details on the emissions setup. Additionally, the complete dataset used in the figures will be made available upon finalization for publication to ensure long-term accessibility and facilitate reproducibility.Additional details
Identifiers
- DOI
- 10.1073/pnas.2506658122
- Other
- oai:uchicago.tind.io:16557
Funding
- European Union
- Horizon 2020 Framework Programme
- European Union
- Marie Skłodowska-Curie Actions Doctoral Network
- Research Council of Finland
- Atmosphere and Climate Competence Center Flagship
- Research Council of Finland
- 337552
- Research Council of Finland
- 337550
- Research Council of Finland
- 302958
- Research Council of Finland
- 1325656
- Research Council of Finland
- 311932
- Research Council of Finland
- 334792
- Research Council of Finland
- 316114
- Research Council of Finland
- 325647
- Research Council of Finland
- 325681
- Research Council of Finland
- 347782
- Research Council of Finland
- 346371
- Research Council of Finland
- 359331
- Jane and Aatos Erkko Foundation
- Jenny ja Antti Wihurin Rahasto
- European Research Council
- 742206
- Research Council of Finland
- 349659
- Bundesministerium für Forschung, Technologie und Raumfahrt
- 01LK2201A
- Bundesministerium für Forschung, Technologie und Raumfahrt
- 01LK2201B
- Bundesministerium für Forschung, Technologie und Raumfahrt
- 01LK2201C
- European Union
- 101056783
- Swiss National Science Foundation
- 200021_213071
- Vienna Science and Technology Fund
- Vienna Science and Technology Fund
- U.S. National Science Foundation
- ATM-2215527
- U.S. National Science Foundation
- AGS-2215522
- U.S. National Science Foundation
- 2027252
- U.S. National Science Foundation
- 2215489
- U.S. National Science Foundation
- 2431817
- U.S. National Science Foundation
- 2132089
- National Aeronautics and Space Administration
- 80NSSC19K0949
- Austrian National Bank
- 2023-5223