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    Modeling dynamic exchange of gaseous elemental mercury at polar sunrise

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    Dastoor(2008).pdf (725.0Kb)
    Authors
    Dastoor, A.P.
    Davignon, D.
    Theys, N.
    Van Roozendael, M.
    Steffen, A.
    Ariya, P.A.
    Show allShow less
    Discipline
    Physical sciences
    Subject
    Atmospheric chemistry
    Atmospherics
    Electron multipliers
    Gems
    Precipitation (meteorology)
    Springs (components)
    Atmospheric concentrations
    Atmospheric mercury
    Gaseous elemental mercury (GEM)
    H igh concentrations
    Mercury chemistry
    Mercury depositions
    Mercury(III)
    Net gain
    Polar Regions
    Rapid cycling
    Re-emission
    Redox transformations
    Satellite data
    Surface exchanges
    Total mercury (Thg)
    Mercury (metal)
    bromine derivative
    halogen
    mercury
    snow
    atmospheric modeling
    flux measurement
    gas exchange
    mercury (element)
    oxidation
    polar region
    satellite data
    air
    Arctic
    article
    atmospheric deposition
    atmospheric dispersion
    model
    oxidation
    oxidation reduction reaction
    spring
    summer
    Air Pollutants
    Arctic Regions
    Mercury
    Periodicity
    Seasons
    Snow
    Sunlight
    Arctic
    Audience
    Scientific
    Date
    2008
    Metadata
    Show full item record
    Description
    At polar sunrise, gaseous elemental mercury (GEM) undergoes an exceptional dynamic exchange in the air and at the snow surface during which GEM can be rapidly removed fromthe atmosphere (the so-called atmospheric mercury depletion events (AMDEs)) as well as re-emitted from the snow within a few hours to days in the Polar Regions. Although high concentrations of total mercury in snow following AMDEs is well documented, there is very little data available on the redox transformation processes of mercury in the snow and the fluxes of mercury at the air/snow interface. Therefore, the net gain of mercury in the Polar Regions as a result of AMDEs is still an open question. We developed a new version of the global mercury model, GRAHM, which includes for the first time bidirectional surface exchange of GEM in Polar Regions in spring and summer by developing schemes for mercury halogen oxidation, deposition, and re-emission. Also for the first time, GOME satellite data-derived boundary layer concentrations of BrO have been used in a global mercury model for representation of halogen mercury chemistry. Comparison of model simulated and measured atmospheric concentrations of GEM at Alert, Canada, for 3 years (2002-2004) shows the model's capability in simulating the rapid cycling of mercury during and after AMDEs. Brooks et al. (1) measured mercury deposition, re-emission, and net surface gain fluxes of mercury at Barrow, AK, during an intensive measurement campaign for a 2 week period in spring (March 25 to April 7, 2003). They reported 1.7, 1.0 ± 0.2, and 0.7 ± 0.2 μg m -2 deposition, re-emission, and net surface gain, respectively. Using the optimal configuration of the model, we estimated 1.8 μg m-2 deposition, 1.0 μg m-2 re-emission, and 0.8 μg m-2 net surface gain of mercury for the same time period at Barrow. The estimated net annual accumulation of mercury within the Arctic Circle north of 66.5° is ∼1741 with ±7 t of interannual variability for 2002-2004 using the optimal configuration. We estimated the uncertainty of the model results to the Hg/Br reaction rate coefficient to be ∼6%. Springtime is clearly demonstrated as the most active period of mercury exchanges and net surface gain (∼46% of annual accumulation) in the Arctic.
    Citation
    Dastoor, A.P.; Davignon, D.; Theys, N.; Van Roozendael, M.; Steffen, A.; Ariya, P.A. (2008). Modeling dynamic exchange of gaseous elemental mercury at polar sunrise. , Environmental Science and Technology, Vol. 42, Issue 14, 5183-5188, DOI: 10.1021/es800291w.
    Identifiers
    uri: https://orfeo.belnet.be/handle/internal/4351
    doi: http://dx.doi.org/10.1021/es800291w
    scopus: 2-s2.0-48249124514
    Type
    Article
    Peer-Review
    No
    Language
    eng
    Links
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