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Titel |
Importance of secondary sources in the atmospheric budgets of formic and acetic acids |
VerfasserIn |
F. Paulot, D. Wunch, J. D. Crounse, G. C. Toon, D. B. Millet, P. F. DeCarlo, C. Vigouroux, N. M. Deutscher, G. González Abad, J. Notholt, T. Warneke, J. W. Hannigan, C. Warneke, J. A. Gouw, E. J. Dunlea, M. Mazière, D. W. T. Griffith, P. Bernath, J. L. Jimenez, P. O. Wennberg |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 11, no. 5 ; Nr. 11, no. 5 (2011-03-04), S.1989-2013 |
Datensatznummer |
250009443
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Publikation (Nr.) |
copernicus.org/acp-11-1989-2011.pdf |
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Zusammenfassung |
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−1, 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. |
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