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Rethinking the global secondary organic aerosol (SOA) budget: Stronger production, faster removal, shorter lifetime

Publication ,  Journal Article
Hodzic, A; Kasibhatla, PS; Jo, DS; Cappa, CD; Jimenez, JL; Madronich, S; Park, RJ
Published in: Atmospheric Chemistry and Physics
June 29, 2016

Recent laboratory studies suggest that secondary organic aerosol (SOA) formation rates are higher than assumed in current models. There is also evidence that SOA removal by dry and wet deposition occurs more efficiently than some current models suggest and that photolysis and heterogeneous oxidation may be important (but currently ignored) SOA sinks. Here, we have updated the global GEOS-Chem model to include this new information on formation (i.e., wall-corrected yields and emissions of semi-volatile and intermediate volatility organic compounds) and on removal processes (photolysis and heterogeneous oxidation). We compare simulated SOA from various model configurations against ground, aircraft and satellite measurements to assess the extent to which these improved representations of SOA formation and removal processes are consistent with observed characteristics of the SOA distribution. The updated model presents a more dynamic picture of the life cycle of atmospheric SOA, with production rates 3.9 times higher and sinks a factor of 3.6 more efficient than in the base model. In particular, the updated model predicts larger SOA concentrations in the boundary layer and lower concentrations in the upper troposphere, leading to better agreement with surface and aircraft measurements of organic aerosol compared to the base model. Our analysis thus suggests that the long-standing discrepancy in model predictions of the vertical SOA distribution can now be resolved, at least in part, by a stronger source and stronger sinks leading to a shorter lifetime. The predicted global SOA burden in the updated model is 0.88Tg and the corresponding direct radiative effect at top of the atmosphere is -0.33Wm-2, which is comparable to recent model estimates constrained by observations. The updated model predicts a population-weighed global mean surface SOA concentration that is a factor of 2 higher than in the base model, suggesting the need for a reanalysis of the contribution of SOA to PM pollution-related human health effects. The potential importance of our estimates highlights the need for more extensive field and laboratory studies focused on characterizing organic aerosol removal mechanisms and rates.

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Published In

Atmospheric Chemistry and Physics

DOI

EISSN

1680-7324

ISSN

1680-7316

Publication Date

June 29, 2016

Volume

16

Issue

12

Start / End Page

7917 / 7941

Related Subject Headings

  • Meteorology & Atmospheric Sciences
  • 3702 Climate change science
  • 3701 Atmospheric sciences
  • 0401 Atmospheric Sciences
  • 0201 Astronomical and Space Sciences
 

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Hodzic, A., Kasibhatla, P. S., Jo, D. S., Cappa, C. D., Jimenez, J. L., Madronich, S., & Park, R. J. (2016). Rethinking the global secondary organic aerosol (SOA) budget: Stronger production, faster removal, shorter lifetime. Atmospheric Chemistry and Physics, 16(12), 7917–7941. https://doi.org/10.5194/acp-16-7917-2016
Hodzic, A., P. S. Kasibhatla, D. S. Jo, C. D. Cappa, J. L. Jimenez, S. Madronich, and R. J. Park. “Rethinking the global secondary organic aerosol (SOA) budget: Stronger production, faster removal, shorter lifetime.” Atmospheric Chemistry and Physics 16, no. 12 (June 29, 2016): 7917–41. https://doi.org/10.5194/acp-16-7917-2016.
Hodzic A, Kasibhatla PS, Jo DS, Cappa CD, Jimenez JL, Madronich S, et al. Rethinking the global secondary organic aerosol (SOA) budget: Stronger production, faster removal, shorter lifetime. Atmospheric Chemistry and Physics. 2016 Jun 29;16(12):7917–41.
Hodzic, A., et al. “Rethinking the global secondary organic aerosol (SOA) budget: Stronger production, faster removal, shorter lifetime.” Atmospheric Chemistry and Physics, vol. 16, no. 12, June 2016, pp. 7917–41. Scopus, doi:10.5194/acp-16-7917-2016.
Hodzic A, Kasibhatla PS, Jo DS, Cappa CD, Jimenez JL, Madronich S, Park RJ. Rethinking the global secondary organic aerosol (SOA) budget: Stronger production, faster removal, shorter lifetime. Atmospheric Chemistry and Physics. 2016 Jun 29;16(12):7917–7941.

Published In

Atmospheric Chemistry and Physics

DOI

EISSN

1680-7324

ISSN

1680-7316

Publication Date

June 29, 2016

Volume

16

Issue

12

Start / End Page

7917 / 7941

Related Subject Headings

  • Meteorology & Atmospheric Sciences
  • 3702 Climate change science
  • 3701 Atmospheric sciences
  • 0401 Atmospheric Sciences
  • 0201 Astronomical and Space Sciences