Published October 27, 2025 | Version v1
Journal article

Global impact of anthropogenic NH3 emissions on upper tropospheric aerosol formation

  • 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

UChicago Information

Division(s)
Physical Sciences Division
Department(s)
Geophysical Sciences