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    Tropospheric bromine chemistry: Implications for present and pre-industrial ozone and mercury

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    Authors
    Parrella, J.P.
    Jacob, D.J.
    Liang, Q.
    Zhang, Y.
    Mickley, L.J.
    Miller, B.
    Evans, M.J.
    Yang, X.
    Pyle, J.A.
    Theys, N.
    Van Roozendael, M.
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    Discipline
    Earth and related Environmental sciences
    Subject
    atmospheric chemistry
    atmospheric modeling
    atmospheric transport
    bromine
    concentration (composition)
    mercury (element)
    ozone
    seasonality
    troposphere
    Arctic
    Atlantic Ocean
    Atlantic Ocean (North)
    Audience
    Scientific
    Date
    2012
    Metadata
    Show full item record
    Description
    We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by <1–8 nmol mol−1 (6.5% globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4%. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40% higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.
    Citation
    Parrella, J.P.; Jacob, D.J.; Liang, Q.; Zhang, Y.; Mickley, L.J.; Miller, B.; Evans, M.J.; Yang, X.; Pyle, J.A.; Theys, N.; Van Roozendael, M. (2012). Tropospheric bromine chemistry: Implications for present and pre-industrial ozone and mercury. , Atmospheric Chemistry and Physics, Vol. 12, Issue 15, 6723-6740, DOI: 10.5194/acp-12-6723-2012.
    Identifiers
    uri: https://orfeo.belnet.be/handle/internal/2985
    doi: http://dx.doi.org/10.5194/acp-12-6723-2012
    scopus: 2-s2.0-84864595860
    Type
    Article
    Peer-Review
    Yes
    Language
    eng
    Links
    NewsHelpdeskBELSPO OA Policy

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