Articles | Volume 17, issue 8
https://doi.org/10.5194/acp-17-5107-2017
https://doi.org/10.5194/acp-17-5107-2017
Research article
 | 
19 Apr 2017
Research article |  | 19 Apr 2017

Inconsistency of ammonium–sulfate aerosol ratios with thermodynamic models in the eastern US: a possible role of organic aerosol

Rachel F. Silvern, Daniel J. Jacob, Patrick S. Kim, Eloise A. Marais, Jay R. Turner, Pedro Campuzano-Jost, and Jose L. Jimenez

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Cited articles

Alexander, B., Park, R. J., Jacob, D. J., Li, Q. B., Yantosca, R. M., Savarino, J., Lee, C. C. W., and Thiemens, M. H.: Sulfate formation in sea-salt aerosols: Constraints from oxygen isotopes, J. Geophys. Res.-Atmos., 110, D10307, https://doi.org/10.1029/2004jd005659, 2005.
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Anttila, T., Kiendler-Scharr, A., Mentel, T. F., and Tillmann, R.: Size dependent partitioning of organic material: evidence for the formation of organic coatings on aqueous aerosols, J. Atmos. Chem., 57, 215–237, https://doi.org/10.1007/s10874-007-9067-9, 2007.
Atmospheric Research and Analysis: SEARCH PM2. 5, available at: http://www.atmospheric-research.com/studies/SEARCH/index.html (last access: 9 August 2016), 2013.
Attwood, A. R., Washenfelder, R. A., Brock, C. A., Hu, W., Baumann, K., Campuzano-Jost, P., Day, D. A., Edgerton, E. S., Murphy, D. M., Palm, B. B., McComiskey, A., Wagner, N. L., de Sa, S. S., Ortega, A., Martin, S. T., Jimenez, J. L., and Brown, S. S.: Trends in sulfate and organic aerosol mass in the Southeast U.S.: Impact on aerosol optical depth and radiative forcing, Geophys. Res. Lett., 41, 7701–7709, https://doi.org/10.1002/2014gl061669, 2014.
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Short summary
We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations of inorganic aerosol composition in the eastern US in summer that shows low ammonium sulfate aerosol ratios. In addition, from 2003 to 2013, while SO2 emissions have declined due to US emission controls, aerosols have become more acidic in the southeastern US. To explain these observations, we suggest that the large and increasing source of organic aerosol may be affecting thermodynamic equilibrium.
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