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10.5194/acpd-7-8663-2007
http://www.atmos-chem-phys-discuss.net/7/8663/2007/
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http://www.atmos-chem-phys-discuss.net/7/8663/2007/acpd-7-8663-2007.pdf
8663
8708
2007-06-21
Retrieval of stratospheric and tropospheric BrO profiles and columns using ground-based zenith-sky DOAS observations at Harestua, 60° N
F. Hendrick
franch@oma.be
M. Van Roozendael
M. P. Chipperfield
M. Dorf
F. Goutail
X. Yang
C. Fayt
C. Hermans
K. Pfeilsticker
J.-P. Pommereau
J. A. Pyle
N. Theys
M. De Mazière
Institut d'Aéronomie Spatiale de Belgique (IASB-BIRA), Brussels, Belgium
Institute for Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
Institute for Environmental Physics, University of Heidelberg, Heidelberg, Germany
Service d'Aéronomie du CNRS, Verrières le Buisson, France
Centre for Atmospheric Science, Department of Chemistry, University of Cambridge, Cambridge, UK
A profiling algorithm based on the optimal estimation method is applied to
ground-based zenith-sky UV-visible measurements from Harestua, Southern
Norway (60° N, 11° E) in order to retrieve BrO vertical profiles. The
sensitivity of the zenith-sky observations to the tropospheric BrO detection
is increased by using for the spectral analysis a constant reference
spectrum corresponding to clear-sky noon summer conditions. The information
content and retrieval errors are characterized and it is shown that the
retrieved stratospheric profiles and total columns are consistent with
correlative balloon and satellite observations, respectively. Tropospheric
BrO columns are derived from profiles retrieved at 80° solar zenith
angle during sunrise and sunset for the 2000–2006 period. They show a marked
seasonality with mean column value ranging from 1.52±0.51×10<sup>13</sup> molec/cm<sup>2</sup> in late winter/early
spring to 0.92±0.31×10<sup>13</sup> molec/cm<sup>2</sup> in summer, which corresponds to 1.0±0.3 and 0.6±0.2 pptv, respectively, if we assume that BrO is uniformly mixed in the
troposphere. These column values are also consistent with previous estimates
made from balloon, satellite, and other ground-based observations. Daytime
(10h30 local time) tropospheric BrO columns are compared to the <i>p</i>-TOMCAT 3-D
tropospheric chemical transport model (CTM) for the 2002–2003 period.
<i>p</i>-TOMCAT shows a good agreement with the retrieved columns except in late
winter/early spring where an underestimation by the model is obtained. This
feature could be explained by the non-inclusion of sea-ice bromine sources
in the current version of <i>p</i>-TOMCAT, which can therefore not reproduce the
possible transport from the polar region to Harestua of air-masses with
enhanced BrO concentration due to bromine explosion events in late
winter/early spring. The corresponding daytime stratospheric BrO columns are
compared to the SLIMCAT 3-D stratospheric CTM. The model run used, which
assumes 21.2 pptv for the Br<sub>y</sub> loading (15 pptv for long-lived bromine
species + 6 extra pptv for very short-lived species (VSLS) added by a
scaling of CH<sub>3</sub>Br), significantly underestimates the retrieved BrO
columns. A sensitivity study shows that a good quantitative agreement can
only be obtained if 8 pptv accounting for VSLS are added directly (and not
by a scaling of CH<sub>3</sub>Br) to the SLIMCAT long-lived bromine species
profile. This contribution of the VSLS to the total bromine loading is also
consistent with recently published studies.
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