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Importance of secondary sources in the atmospheric budgets of formic and acetic acids

Journal Article


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Abstract


  • We present a detailed budget of formic and acetic acids, two of the most abundant trace gases in the atmosphere. Our bottom-up estimate of the global source of formic and acetic acids are ∼1200 and ∼1400 Gmol/yr, dominated by photochemical oxidation of biogenic volatile organic compounds, in particular isoprene. Their sinks are dominated by wet and dry deposition. We use the GEOS-Chem chemical transport model to evaluate this budget against an extensive suite of measurements from ground, ship and satellite-based Fourier transform spectrometers, as well as from several aircraft campaigns over North America. The model captures the seasonality of formic and acetic acids well but generally underestimates their concentration, particularly in the Northern midlatitudes. We infer that the source of both carboxylic acids may be up to 50% greater than our estimate and report evidence for a long-lived missing secondary source of carboxylic acids that may be associated with the aging of organic aerosols. Vertical profiles of formic acid in the upper troposphere support a negative temperature dependence of the reaction between formic acid and the hydroxyl radical as suggested by several theoretical studies. © Author(s) 2010.

UOW Authors


  •   Paulot, Fabien (external author)
  •   Wunch, Debra (external author)
  •   Crounse, John D. (external author)
  •   Toon, Geoffrey C. (external author)
  •   Millet, Dylan B. (external author)
  •   DeCarlo, Peter F. (external author)
  •   Vigouroux, C (external author)
  •   Deutscher, Nicholas
  •   Gonzalez Abad, G (external author)
  •   Notholt, Justus (external author)
  •   Warneke, Thorsten (external author)
  •   Hannigan, J W. (external author)
  •   Warneke, Carsten (external author)
  •   De Gouw, Joost A. (external author)
  •   Dunlea, Edward (external author)
  •   de Maziere, M (external author)
  •   Griffith, David
  •   Bernath, Peter (external author)
  •   Jimenez, Jose L. (external author)
  •   Wennberg, Paul O. (external author)

Publication Date


  • 2010

Citation


  • Paulot, F., Wunch, D., Crounse, J. D., Toon, G., Millet, D. B., DeCarlo, P. F., Vigouroux, C., Deutscher, N. M., Gonzalez Abad, G., Notholt, J., Warneke, T., Hannigan, J., Warneke, C., De Gouw, J. A., Dunlea, E., De Maziere, M., Griffith, D. W., Bernath, P., Jimenez, J. L. & Wennberg, P. O. (2010). Importance of secondary sources in the atmospheric budgets of formic and acetic acids. Atmospheric Chemistry and Physics Discussions, 10 (10), 24435-24498.

Scopus Eid


  • 2-s2.0-79952342467

Ro Full-text Url


  • http://ro.uow.edu.au/cgi/viewcontent.cgi?article=1650&context=scipapers

Ro Metadata Url


  • http://ro.uow.edu.au/scipapers/611

Has Global Citation Frequency


Number Of Pages


  • 63

Start Page


  • 24435

End Page


  • 24498

Volume


  • 10

Issue


  • 10

Abstract


  • We present a detailed budget of formic and acetic acids, two of the most abundant trace gases in the atmosphere. Our bottom-up estimate of the global source of formic and acetic acids are ∼1200 and ∼1400 Gmol/yr, dominated by photochemical oxidation of biogenic volatile organic compounds, in particular isoprene. Their sinks are dominated by wet and dry deposition. We use the GEOS-Chem chemical transport model to evaluate this budget against an extensive suite of measurements from ground, ship and satellite-based Fourier transform spectrometers, as well as from several aircraft campaigns over North America. The model captures the seasonality of formic and acetic acids well but generally underestimates their concentration, particularly in the Northern midlatitudes. We infer that the source of both carboxylic acids may be up to 50% greater than our estimate and report evidence for a long-lived missing secondary source of carboxylic acids that may be associated with the aging of organic aerosols. Vertical profiles of formic acid in the upper troposphere support a negative temperature dependence of the reaction between formic acid and the hydroxyl radical as suggested by several theoretical studies. © Author(s) 2010.

UOW Authors


  •   Paulot, Fabien (external author)
  •   Wunch, Debra (external author)
  •   Crounse, John D. (external author)
  •   Toon, Geoffrey C. (external author)
  •   Millet, Dylan B. (external author)
  •   DeCarlo, Peter F. (external author)
  •   Vigouroux, C (external author)
  •   Deutscher, Nicholas
  •   Gonzalez Abad, G (external author)
  •   Notholt, Justus (external author)
  •   Warneke, Thorsten (external author)
  •   Hannigan, J W. (external author)
  •   Warneke, Carsten (external author)
  •   De Gouw, Joost A. (external author)
  •   Dunlea, Edward (external author)
  •   de Maziere, M (external author)
  •   Griffith, David
  •   Bernath, Peter (external author)
  •   Jimenez, Jose L. (external author)
  •   Wennberg, Paul O. (external author)

Publication Date


  • 2010

Citation


  • Paulot, F., Wunch, D., Crounse, J. D., Toon, G., Millet, D. B., DeCarlo, P. F., Vigouroux, C., Deutscher, N. M., Gonzalez Abad, G., Notholt, J., Warneke, T., Hannigan, J., Warneke, C., De Gouw, J. A., Dunlea, E., De Maziere, M., Griffith, D. W., Bernath, P., Jimenez, J. L. & Wennberg, P. O. (2010). Importance of secondary sources in the atmospheric budgets of formic and acetic acids. Atmospheric Chemistry and Physics Discussions, 10 (10), 24435-24498.

Scopus Eid


  • 2-s2.0-79952342467

Ro Full-text Url


  • http://ro.uow.edu.au/cgi/viewcontent.cgi?article=1650&context=scipapers

Ro Metadata Url


  • http://ro.uow.edu.au/scipapers/611

Has Global Citation Frequency


Number Of Pages


  • 63

Start Page


  • 24435

End Page


  • 24498

Volume


  • 10

Issue


  • 10