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    Airborne DOAS limb measurements of tropospheric trace gas profiles: Case studies on the profile retrieval of O 4 and BrO

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    Authors
    Prados-Roman, C.
    Butz, A.
    Deutschmann, T.
    Dorf, M.
    Kritten, L.
    Minikin, A.
    Platt, U.
    Schlager, H.
    Sihler, H.
    Theys, N.
    Van Roozendael, M.
    Wagner, T.
    Pfeilsticker, K.
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    Discipline
    Earth and related Environmental sciences
    Subject
    aircraft
    algorithm
    atmospheric chemistry
    balloon observation
    cloud radiative forcing
    halogen
    mixing ratio
    ozone
    radiative transfer
    radical
    spatiotemporal analysis
    spectrometer
    stratosphere-troposphere interaction
    trace gas
    ultraviolet radiation
    vertical profile
    visible spectrum
    Arctic
    Svalbard
    Svalbard and Jan Mayen
    Falconidae
    Audience
    Scientific
    Date
    2011
    Metadata
    Show full item record
    Description
    A novel limb scanning mini-DOAS spectrometer for the detection of UV/vis absorbing radicals (e.g., O3, BrO, IO, HONO) was deployed on the DLR-Falcon (Deutsches Zentrum für Luft- und Raumfahrt) aircraft and tested during the ASTAR 2007 campaign (Arctic Study of Tropospheric Aerosol, Clouds and Radiation) that took place at Svalbard (78° N) in spring 2007. Our main objectives during this campaign were to test the instrument, and to perform spectral and profile retrievals of tropospheric trace gases, with particular interest on investigating the distribution of halogen compounds (e.g., BrO) during the so-called ozone depletion events (ODEs). In the present work, a new method for the retrieval of vertical profiles of tropospheric trace gases from tropospheric DOAS limb observations is presented. Major challenges arise from modeling the radiative transfer in an aerosol and cloud particle loaded atmosphere, and from overcoming the lack of a priori knowledge of the targeted trace gas vertical distribution (e.g., unknown tropospheric BrO vertical distribution). Here, those challenges are tackled by a mathematical inversion of tropospheric trace gas profiles using a regularization approach constrained by a retrieved vertical profile of the aerosols extinction coefficient EM. The validity and limitations of the algorithm are tested with in situ measured EM, and with an absorber of known vertical profile (O4). The method is then used for retrieving vertical profiles of tropospheric BrO. Results indicate that, for aircraft ascent/descent observations, the limit for the BrO detection is roughly 1.5 pptv (pmol mol−1), and the BrO profiles inferred from the boundary layer up to the upper troposphere and lower stratosphere have around 10 degrees of freedom. For the ASTAR 2007 deployments during ODEs, the retrieved BrO vertical profiles consistently indicate high BrO mixing ratios (∼15 pptv) within the boundary layer, low BrO mixing ratios (≤1.5 pptv) in the free troposphere, occasionally enhanced BrO mixing ratios (∼1.5 pptv) in the upper troposphere, and increasing BrO mixing ratios with altitude in the lowermost stratosphere. These findings agree reasonably well with satellite and balloon-borne soundings of total and partial BrO atmospheric column densities.
    Citation
    Prados-Roman, C.; Butz, A.; Deutschmann, T.; Dorf, M.; Kritten, L.; Minikin, A.; Platt, U.; Schlager, H.; Sihler, H.; Theys, N.; Van Roozendael, M.; Wagner, T.; Pfeilsticker, K. (2011). Airborne DOAS limb measurements of tropospheric trace gas profiles: Case studies on the profile retrieval of O 4 and BrO. , Atmospheric Measurement Techniques, Vol. 4, Issue 6, 1241-1260, DOI: 10.5194/amt-4-1241-2011.
    Identifiers
    uri: https://orfeo.belnet.be/handle/internal/3117
    doi: http://dx.doi.org/10.5194/amt-4-1241-2011
    scopus: 2-s2.0-80052691138
    Type
    Article
    Peer-Review
    Yes
    Language
    eng
    Links
    NewsHelpdeskBELSPO OA Policy

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