Chemical transport models often underestimate inorganic aerosol acidity in remote regions of the atmosphere

The inorganic fraction of fine particles affects numerous physicochemical processes in the atmosphere. However, there is large uncertainty in its burden and composition due to limited global measurements. Here, we present observations from eleven different aircraft campaigns from around the globe and investigate how aerosol pH and ammonium balance change from polluted to remote regions, such as over the oceans. Both parameters show increasing acidity with remoteness, at all altitudes, with pH decreasing from about 3 to about −1 and ammonium balance decreasing from almost 1 to nearly 0. We compare these observations against nine widely used chemical transport models and find that the simulations show more scatter (generally R2 < 0.50) and typically predict less acidic aerosol in the most remote regions. These differences in observations and predictions are likely to result in underestimating the model-predicted direct radiative cooling effect for sulfate, nitrate, and ammonium aerosol by 15–39%.

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Author Nault, Benjamin A.
Campuzano-Jost, Pedro
Day, Douglas A.
Jo, Duseong S.
Schroder, Jason C.
Allen, Hannah M.
Bahreini, Roya
Bian, Huisheng
Blake, Donald R.
Chin, Mian
Clegg, Simon L.
Colarco, Peter R.
Crounse, John D.
Cubison, Michael J.
DeCarlo, Peter F.
Dibb, Jack E.
Diskin, Glenn S.
Hodzic, Alma
Hu, Weiwei
Katich, Joseph M.
Kim, Michelle J.
Kodros, John K.
Kupc, Agnieszka
Lopez-Hilfiker, Felipe D.
Marais, Eloise A.
Middlebrook, Ann M.
Andrew Neuman, J.
Nowak, John B.
Palm, Brett B.
Paulot, Fabien
Pierce, Jeffrey R.
Schill, Gregory P.
Scheuer, Eric
Thornton, Joel A.
Tsigaridis, Kostas
Wennberg, Paul O.
Williamson, Christina J.
Jimenez, Jose L.
Publisher UCAR/NCAR - Library
Publication Date 2021-12-14T00:00:00
Digital Object Identifier (DOI) Not Assigned
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Resource Version N/A
Topic Category geoscientificInformation
Progress N/A
Metadata Date 2023-08-18T18:29:11.294997
Metadata Record Identifier edu.ucar.opensky::articles:24419
Metadata Language eng; USA
Suggested Citation Nault, Benjamin A., Campuzano-Jost, Pedro, Day, Douglas A., Jo, Duseong S., Schroder, Jason C., Allen, Hannah M., Bahreini, Roya, Bian, Huisheng, Blake, Donald R., Chin, Mian, Clegg, Simon L., Colarco, Peter R., Crounse, John D., Cubison, Michael J., DeCarlo, Peter F., Dibb, Jack E., Diskin, Glenn S., Hodzic, Alma, Hu, Weiwei, Katich, Joseph M., Kim, Michelle J., Kodros, John K., Kupc, Agnieszka, Lopez-Hilfiker, Felipe D., Marais, Eloise A., Middlebrook, Ann M., Andrew Neuman, J., Nowak, John B., Palm, Brett B., Paulot, Fabien, Pierce, Jeffrey R., Schill, Gregory P., Scheuer, Eric, Thornton, Joel A., Tsigaridis, Kostas, Wennberg, Paul O., Williamson, Christina J., Jimenez, Jose L.. (2021). Chemical transport models often underestimate inorganic aerosol acidity in remote regions of the atmosphere. UCAR/NCAR - Library. http://n2t.net/ark:/85065/d79z989b. Accessed 07 February 2025.

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