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First remote sensing measurements of ClOOCl along with ClO and ClONO2 in activated and deactivated Arctic vortex conditions using new ClOOCl IR absorption cross sections

Wetzel, G. and Oelhaf, H. and Kirner, O. and Ruhnke, R. and Friedl-Vallon, F. and Kleinert, A. and Maucher, G. and Fischer, H. and Birk, Manfred and Wagner, Georg and Engel, A. (2010) First remote sensing measurements of ClOOCl along with ClO and ClONO2 in activated and deactivated Arctic vortex conditions using new ClOOCl IR absorption cross sections. Atmospheric Chemistry and Physics, 10, pp. 931-945. Copernicus Publications on behalf of the European Geosciences Union.

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Abstract

Abstract. Active chlorine species play a dominant role in the catalytic destruction of stratospheric ozone in the polar vortices during the late winter and early spring seasons. Recently, the correct understanding of the ClO dimer cycle was challenged by the release of new laboratory absorption cross sections (Pope et al., 2007) yielding significant model underestimates of observed ClO and ozone loss (von Hobe et al., 2007). Under this aspect, nocturnal Arctic stratospheric limb emission measurements carried out by the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 11 January 2001 and 20/21 March 2003 have been reanalyzed with regard to the chlorine reservoir species ClONO2 and the active species, ClO and ClOOCl (Cl2O2). New laboratory measurements of IR absorption cross sections of ClOOCl for various temperatures and pressures allowed for the first time the retrieval of ClOOCl mixing ratios from remote sensing measurements. High values of active chlorine (ClOx) of roughly 2.3 ppbv at 20 km were observed by MIPAS-B in the cold mid-winter Arctic vortex on 11 January 2001. While nighttime ClOOCl shows enhanced values of nearly 1.1 ppbv at 20 km, ClONO2 mixing ratios are less than 0.1 ppbv at this altitude. In contrast, high ClONO2 mixing ratios of nearly 2.4 ppbv at 20 km have been observed in the late winter Arctic vortex on 20 March 2003. No significant ClOx amounts are detectable on this date since most of the active chlorine has already recovered to its main reservoir species ClONO2. The observed values of ClOx and ClONO2 are in line with the established polar chlorine chemistry. The thermal equilibrium constants between the dimer formation and its dissociation, as derived from the balloon measurements, are on the lower side of reported data and in good agreement with values recommended by von Hobe et al. (2007). Calculations with the ECHAM/MESSy Atmospheric Chemistry model (EMAC) using established kinetics show similar chlorine activation and deactivation, compared to the measurements in January 2001 and March 2003, respectively.

Document Type:Article
Title:First remote sensing measurements of ClOOCl along with ClO and ClONO2 in activated and deactivated Arctic vortex conditions using new ClOOCl IR absorption cross sections
Authors:
AuthorsInstitution or Email of Authors
Wetzel, G.Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
Oelhaf, H.Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
Kirner, O.Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
Ruhnke, R.Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
Friedl-Vallon, F.Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
Kleinert, A.Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
Maucher, G.Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
Fischer, H.Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany
Birk, Manfredmanfred.birk@dlr.de
Wagner, Georggeorg.wagner@dlr.de
Engel, A.Institut für Atmosphäre und Umwelt, J. W. Goethe Universität Frankfurt, Frankfurt, Germany
Date:2010
Journal or Publication Title:Atmospheric Chemistry and Physics
Refereed publication:Yes
In Open Access:Yes
In SCOPUS:Yes
In ISI Web of Science:Yes
Volume:10
Page Range:pp. 931-945
Publisher:Copernicus Publications on behalf of the European Geosciences Union
Status:Published
Keywords:atmospheric remote sensing, MIPAS-B, chlorine, ClOOCl, ClO dimer, chlorine peroxide, infrared absorption cross sections, arctic perturbed chemistry
HGF - Research field:Aeronautics, Space and Transport (old)
HGF - Program:Space (old)
HGF - Program Themes:W EO - Erdbeobachtung
DLR - Research area:Space
DLR - Program:W EO - Erdbeobachtung
DLR - Research theme (Project):W - Vorhaben Spektrometrische Verfahren und Konzepte der Fernerkundung (old)
Location: Oberpfaffenhofen
Institutes and Institutions:Remote Sensing Technology Institute > Experimental Methods
Deposited By: Dr.rer.nat. Georg Wagner
Deposited On:05 Jul 2010 10:13
Last Modified:12 Dec 2013 20:58

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