Chemical transport models often underestimate inorganic aerosol acidity in remote regions of the atmosphere
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Published:2021-05-14
Issue:1
Volume:2
Page:
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ISSN:2662-4435
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Container-title:Communications Earth & Environment
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language:en
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Short-container-title:Commun Earth Environ
Author:
Nault Benjamin A.ORCID, Campuzano-Jost PedroORCID, Day Douglas A., Jo Duseong S.ORCID, Schroder Jason C., Allen Hannah M., Bahreini RoyaORCID, Bian Huisheng, Blake Donald R., Chin MianORCID, Clegg Simon L., Colarco Peter R.ORCID, Crounse John D.ORCID, Cubison Michael J., DeCarlo Peter F.ORCID, Dibb Jack E.ORCID, Diskin Glenn S.ORCID, Hodzic Alma, Hu Weiwei, Katich Joseph M., Kim Michelle J., Kodros John K.ORCID, Kupc AgnieszkaORCID, Lopez-Hilfiker Felipe D., Marais Eloise A.ORCID, Middlebrook Ann M.ORCID, Andrew Neuman J., Nowak John B.ORCID, Palm Brett B.ORCID, Paulot FabienORCID, Pierce Jeffrey R.ORCID, Schill Gregory P.ORCID, Scheuer Eric, Thornton Joel A., Tsigaridis KostasORCID, Wennberg Paul O.ORCID, Williamson Christina J.ORCID, Jimenez Jose L.ORCID
Abstract
AbstractThe 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%.
Publisher
Springer Science and Business Media LLC
Subject
General Earth and Planetary Sciences,General Environmental Science
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