Concentrations and sources of organic carbon aerosols in the free troposphere over North America

Colette L. Heald, Daniel J. Jacob, Solène Turquety, Rynda C. Hudman, Rodney J. Weber, Amy P. Sullivan, Richard E. Peltier, Elliot L Atlas, Joost A. de Gouw, Carsten Warneke, John S. Holloway, Andrew Neuman, Frank M. Flocke, John H. Seinfeld

Research output: Contribution to journalArticle

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Abstract

Aircraft measurements of water-soluble organic carbon (WSOC) aerosol over NE North America during summer 2004 (ITCT-2K4) are simulated with a global chemical transport model (GEOS-Chem) to test our understanding of the sources of organic carbon (OC) aerosol in the free troposphere (FT). Elevated concentrations were observed in plumes from boreal fires in Alaska and Canada. WSOC aerosol concentrations outside of these plumes average 0.9 ± 0.9 μg C m-3 in the FT (2-6 km). The corresponding model value is 0.7 ± 0.6 μg C m-3, including 42% from biomass burning, 36% from biogenic secondary organic aerosol (SOA), and 22% from anthropogenic emissions. Previous OC aerosol observations over the NW Pacific in spring 2001 (ACE-Asia) averaged 3.3 ± 2.8 μg C m-3 in the FT, compared to a model value of 0.3 ± 0.3 μg C m-3. WSOC aerosol concentrations in the boundary layer (BL) during ITCT-2K4 are consistent with OC aerosol observed at the IMPROVE surface network. The model is low in the boundary layer by 30%, which we attribute to secondary formation at a rate comparable to primary anthropogenic emission. Observed WSOC aerosol concentrations decrease by a factor of 2 from the BL to the FT, as compared to a factor of 10 decrease for sulfate, indicating that most of the WSOC aerosol in the FT originates in situ. Despite reproducing mean observed WSOC concentrations in the FT to within 25%, the model cannot account for the variance in the observations (R = 0.21). Covariance analysis of FT WSOC aerosol with other measured chemical variables suggests an aqueous-phase mechanism for SOA generation involving biogenic precursors.

Original languageEnglish (US)
Article numberD23S47
JournalJournal of Geophysical Research C: Oceans
Volume111
Issue number23
DOIs
StatePublished - Dec 16 2006

Fingerprint

Troposphere
Organic carbon
troposphere
Aerosols
aerosols
organic carbon
aerosol
carbon
Water
water
boundary layers
Boundary layers
boundary layer
plumes
North America
plume
biomass burning
covariance analysis
airborne survey
EOS

ASJC Scopus subject areas

  • Geochemistry and Petrology
  • Geophysics
  • Earth and Planetary Sciences (miscellaneous)
  • Space and Planetary Science
  • Atmospheric Science
  • Astronomy and Astrophysics
  • Oceanography

Cite this

Heald, C. L., Jacob, D. J., Turquety, S., Hudman, R. C., Weber, R. J., Sullivan, A. P., ... Seinfeld, J. H. (2006). Concentrations and sources of organic carbon aerosols in the free troposphere over North America. Journal of Geophysical Research C: Oceans, 111(23), [D23S47]. https://doi.org/10.1029/2005JD007705

Concentrations and sources of organic carbon aerosols in the free troposphere over North America. / Heald, Colette L.; Jacob, Daniel J.; Turquety, Solène; Hudman, Rynda C.; Weber, Rodney J.; Sullivan, Amy P.; Peltier, Richard E.; Atlas, Elliot L; de Gouw, Joost A.; Warneke, Carsten; Holloway, John S.; Neuman, Andrew; Flocke, Frank M.; Seinfeld, John H.

In: Journal of Geophysical Research C: Oceans, Vol. 111, No. 23, D23S47, 16.12.2006.

Research output: Contribution to journalArticle

Heald, CL, Jacob, DJ, Turquety, S, Hudman, RC, Weber, RJ, Sullivan, AP, Peltier, RE, Atlas, EL, de Gouw, JA, Warneke, C, Holloway, JS, Neuman, A, Flocke, FM & Seinfeld, JH 2006, 'Concentrations and sources of organic carbon aerosols in the free troposphere over North America', Journal of Geophysical Research C: Oceans, vol. 111, no. 23, D23S47. https://doi.org/10.1029/2005JD007705
Heald, Colette L. ; Jacob, Daniel J. ; Turquety, Solène ; Hudman, Rynda C. ; Weber, Rodney J. ; Sullivan, Amy P. ; Peltier, Richard E. ; Atlas, Elliot L ; de Gouw, Joost A. ; Warneke, Carsten ; Holloway, John S. ; Neuman, Andrew ; Flocke, Frank M. ; Seinfeld, John H. / Concentrations and sources of organic carbon aerosols in the free troposphere over North America. In: Journal of Geophysical Research C: Oceans. 2006 ; Vol. 111, No. 23.
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abstract = "Aircraft measurements of water-soluble organic carbon (WSOC) aerosol over NE North America during summer 2004 (ITCT-2K4) are simulated with a global chemical transport model (GEOS-Chem) to test our understanding of the sources of organic carbon (OC) aerosol in the free troposphere (FT). Elevated concentrations were observed in plumes from boreal fires in Alaska and Canada. WSOC aerosol concentrations outside of these plumes average 0.9 ± 0.9 μg C m-3 in the FT (2-6 km). The corresponding model value is 0.7 ± 0.6 μg C m-3, including 42{\%} from biomass burning, 36{\%} from biogenic secondary organic aerosol (SOA), and 22{\%} from anthropogenic emissions. Previous OC aerosol observations over the NW Pacific in spring 2001 (ACE-Asia) averaged 3.3 ± 2.8 μg C m-3 in the FT, compared to a model value of 0.3 ± 0.3 μg C m-3. WSOC aerosol concentrations in the boundary layer (BL) during ITCT-2K4 are consistent with OC aerosol observed at the IMPROVE surface network. The model is low in the boundary layer by 30{\%}, which we attribute to secondary formation at a rate comparable to primary anthropogenic emission. Observed WSOC aerosol concentrations decrease by a factor of 2 from the BL to the FT, as compared to a factor of 10 decrease for sulfate, indicating that most of the WSOC aerosol in the FT originates in situ. Despite reproducing mean observed WSOC concentrations in the FT to within 25{\%}, the model cannot account for the variance in the observations (R = 0.21). Covariance analysis of FT WSOC aerosol with other measured chemical variables suggests an aqueous-phase mechanism for SOA generation involving biogenic precursors.",
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