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Diurnal variations of reactive chlorine and nitrogen oxides observed by MIPAS-B inside the January 2010 Arctic vortex

Author(s): G. Wetzel | H. Oelhaf | F. Friedl-Vallon | O. Kirner | A. Kleinert | G. Maucher | H. Nordmeyer | J. Orphal | R. Ruhnke

Journal: Atmospheric Chemistry and Physics Discussions
ISSN 1680-7367

Volume: 12;
Issue: 2;
Start page: 4867;
Date: 2012;
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The winter 2009/2010 was characterized by a strong Arctic vortex with extremely cold mid-winter temperatures in the lower stratosphere associated with an intense activation of reactive chlorine compounds (ClOx). In order to assess the capacities of state-of-the-art chemistry models to predict polar stratospheric chemistry, stratospheric limb emission spectra were recorded during a flight of the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 24 January 2010 inside the Arctic vortex. Several fast limb sequences of spectra (in time steps of about 10 min) were measured from nighttime photochemical equilibrium to local noon allowing the retrieval of chlorine- and nitrogen-containing species which change quickly their concentration around the terminator between night and day. Mixing ratios of species like ClO, NO2, and N2O5 show significant changes around sunrise, which are temporally delayed due to shadowing of the lower stratosphere by upper tropospheric and polar stratospheric clouds. ClO variations were derived for the first time from MIPAS-B spectra. Daytime ClO values of up to 1.6 ppbv are visible in a broad chlorine activated layer below 26 km correlated with low values (close to zero) of its reservoir species ClONO2. Observations are compared and discussed with calculations performed with the 3-dimensional Chemistry Climate Model EMAC (ECHAM5/MESSy Atmospheric Chemistry). Mixing ratios of the species ClO, NO2, and N2O5 are fairly well reproduced by the model during photochemical equilibrium. However, since the model assumes cloudless illumination, simulated concentration changes around sunrise start earlier but less quickly compared to the observed variation of the species concentration.
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