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    Latitudinal and vertical distribution of bromine monoxide in the lower stratosphere from Scanning Imaging Absorption Spectrometer for Atmospheric Chartography limb scattering measurements

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    Authors
    Sioris, C.E.
    Kovalenko, L.J.
    McLinden, C.A.
    Salawitch, R.J.
    Van Roozendael, M.
    Goutail, F.
    Dorf, M.
    Pfeilsticker, K.
    Chance, K.
    von Savigny, C.
    Liu, X.
    Kurosu, T.P.
    Pommereau, J.-P.
    Bösch, H.
    Frerick, J.
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    Discipline
    Earth and related Environmental sciences
    Subject
    Atmospheric chemistry
    Atmospheric humidity
    Bromine compounds
    Spectrometers
    Upper atmosphere
    atomic absorption spectroscopy
    balloon observation
    bromine compound
    imaging method
    latitudinal gradient
    mixing ratio
    scattering
    stratosphere
    vertical distribution
    vertical profile
    Audience
    Scientific
    Date
    2006
    Metadata
    Show full item record
    Description
    Vertical profiles of stratospheric bromine monoxide (BrO) in the 15-30 km range are retrieved from SCIAMACHY limb scatter data over the globe. First validation comparisons with the balloon-borne SAOZ-BrO and LPMA/DOAS instruments indicate retrieval biases of ∼20% or less. Propagated spectral fitting uncertainties lead to a precision approaching ∼25% on a 2 km grid at 25 km. This worsens at higher altitudes because of reduced signal and at lower altitudes because of the reduced penetrability of the atmosphere. In terms of volume mixing ratio (VMR), the single profile precision increases from ∼4 pptv at 17 km to ∼8 pptv at 27 km. Repeatability, an alternative indicator of precision, is 2-3 pptv for SCIAMACHY retrievals and independent of altitude. The BrO stratospheric number density peak generally lies 5 ± 2 km above the tropopause. In the tropics, the stratospheric BrO VMR generally increases with increasing altitude. The observed stratospheric BrO global distribution is generally consistent with previous balloon measurements but does not agree well with results of a model that uses Bry inferred only from the observed breakdown of long-lived bromoalkanes (i.e., methyl bromide and halons). We find best agreement with the observed vertical and latitudinal distribution of BrO for model results that include an 8.4 ± 2 pptv contribution to stratospheric Bry, most of which is expected from the breakdown of VSL (very short lived) bromocarbons, in addition to the ∼16 pptv contribution from longer-lived sources. This suggests that stratospheric Bry exceeds 20 pptv. Profiles of Bry profiles derived from the balloon measurements of BrO also suggest Bry is in excess of 20 pptv, but the uncertainty and variability of these results do not allow us to definitively rule out this concentration. We find typical BrO VMRs of ∼4 pptv at 15 km in the tropical tropopause layer, suggesting that a significant portion of the bromine from VSL bromoalkane sources may be carried across the tropopause in the form of inorganic decomposition products. We discuss a variety of VSL bromocarbons species that may be contributing to the elevated concentrations of stratospheric BrO.
    Citation
    Sioris, C.E.; Kovalenko, L.J.; McLinden, C.A.; Salawitch, R.J.; Van Roozendael, M.; Goutail, F.; Dorf, M.; Pfeilsticker, K.; Chance, K.; von Savigny, C.; Liu, X.; Kurosu, T.P.; Pommereau, J.-P.; Bösch, H.; Frerick, J. (2006). Latitudinal and vertical distribution of bromine monoxide in the lower stratosphere from Scanning Imaging Absorption Spectrometer for Atmospheric Chartography limb scattering measurements. , Journal of Geophysical Research Atmospheres, Vol. 111, Issue 14, D14301, DOI: 10.1029/2005JD006479.
    Identifiers
    uri: https://orfeo.belnet.be/handle/internal/4501
    doi: http://dx.doi.org/10.1029/2005JD006479
    scopus: 2-s2.0-33845660532
    Type
    Article
    Peer-Review
    Yes
    Language
    eng
    Links
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