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

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    Authors
    Paulot, F.
    Wunch, D.
    Crounse, J.D.
    Toon, G.C.
    Millet, D.B.
    Decarlo, P.F.
    Vigouroux, C.
    Deutscher, N.M.
    Abad, G.G.
    Notholt, J.
    Warneke, T.
    Hannigan, J.W.
    Warneke, C.
    De Gouw, J.A.
    Dunlea, E.J.
    De Maziere, M.
    Griffith, D.W.T.
    Bernath, P.
    Jimenez, J.L.
    Wennberg, P.O.
    Show allShow less
    Discipline
    Earth and related Environmental sciences
    Subject
    acetic acid
    atmospheric chemistry
    dry deposition
    formic acid
    hydroxyl radical
    numerical model
    photochemistry
    source-sink dynamics
    troposphere
    vertical profile
    wet deposition
    North America
    Audience
    Scientific
    Date
    2011
    Metadata
    Show full item record
    Description
    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.
    Citation
    Paulot, F.; Wunch, D.; Crounse, J.D.; Toon, G.C.; Millet, D.B.; Decarlo, P.F.; Vigouroux, C.; Deutscher, N.M.; Abad, G.G.; Notholt, J.; Warneke, T.; Hannigan, J.W.; Warneke, C.; De Gouw, J.A.; Dunlea, E.J.; De Maziere, M.; Griffith, D.W.T.; Bernath, P.; Jimenez, J.L.; Wennberg, P.O. (2011). Importance of secondary sources in the atmospheric budgets of formic and acetic acids. , Atmospheric Chemistry and Physics, Vol. 11, Issue 5, 1989-2013, DOI: 10.5194/acp-11-1989-2011.
    Identifiers
    uri: https://orfeo.belnet.be/handle/internal/3112
    doi: http://dx.doi.org/10.5194/acp-11-1989-2011
    Type
    Article
    Peer-Review
    Yes
    Language
    eng
    Links
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