Atmos. Chem. Phys., 12, 8851-8864, 2012
www.atmos-chem-phys.net/12/8851/2012/
doi:10.5194/acp-12-8851-2012
© Author(s) 2012. This work is distributed
under the Creative Commons Attribution 3.0 License.
Analysis of stratospheric NO2 trends above Jungfraujoch using ground-based UV-visible, FTIR, and satellite nadir observations
F. Hendrick1, E. Mahieu2, G. E. Bodeker3, K. F. Boersma4,5, M. P. Chipperfield6, M. De Mazière1, I. De Smedt1, P. Demoulin2, C. Fayt1, C. Hermans1, K. Kreher7, B. Lejeune2, G. Pinardi1, C. Servais2, R. Stübi8, R. van der A4, J.-P. Vernier9,10, and M. Van Roozendael1
1Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, Belgium
2Institute of Astrophysics and Geophysics of the University of Liège, Liège, Belgium
3Bodeker Scientific, Alexandra, New Zealand
4Royal Netherlands Meteorological Institute (KNMI), De Bilt, The Netherlands
5Eindhoven University of Technology, Eindhoven, The Netherlands
6School of Earth and Environment, University of Leeds, Leeds, UK
7National Institute of Water and Atmospheric Research, Omakau, Central Otago, New Zealand
8MeteoSwiss, Payerne, Switzerland
9Science Systems and Applications, Inc., Hampton, Virginia, USA
10NASA Langley Research Center, Hampton, Virginia, USA

Abstract. The trend in stratospheric NO2 column at the NDACC (Network for the Detection of Atmospheric Composition Change) station of Jungfraujoch (46.5° N, 8.0° E) is assessed using ground-based FTIR and zenith-scattered visible sunlight SAOZ measurements over the period 1990 to 2009 as well as a composite satellite nadir data set constructed from ERS-2/GOME, ENVISAT/SCIAMACHY, and METOP-A/GOME-2 observations over the 1996–2009 period. To calculate the trends, a linear least squares regression model including explanatory variables for a linear trend, the mean annual cycle, the quasi-biennial oscillation (QBO), solar activity, and stratospheric aerosol loading is used. For the 1990–2009 period, statistically indistinguishable trends of −3.7 ± 1.1% decade−1 and −3.6 ± 0.9% decade−1 are derived for the SAOZ and FTIR NO2 column time series, respectively. SAOZ, FTIR, and satellite nadir data sets show a similar decrease over the 1996–2009 period, with trends of −2.4 ± 1.1% decade−1, −4.3 ± 1.4% decade−1, and −3.6 ± 2.2% decade−1, respectively. The fact that these declines are opposite in sign to the globally observed +2.5% decade−1 trend in N2O, suggests that factors other than N2O are driving the evolution of stratospheric NO2 at northern mid-latitudes. Possible causes of the decrease in stratospheric NO2 columns have been investigated. The most likely cause is a change in the NO2/NO partitioning in favor of NO, due to a possible stratospheric cooling and a decrease in stratospheric chlorine content, the latter being further confirmed by the negative trend in the ClONO2 column derived from FTIR observations at Jungfraujoch. Decreasing ClO concentrations slows the NO + ClO → NO2 + Cl reaction and a stratospheric cooling slows the NO + O3 → NO2 + O2 reaction, leaving more NOx in the form of NO. The slightly positive trends in ozone estimated from ground- and satellite-based data sets are also consistent with the decrease of NO2 through the NO2 + O3 → NO3 + O2 reaction. Finally, we cannot rule out the possibility that a strengthening of the Dobson-Brewer circulation, which reduces the time available for N2O photolysis in the stratosphere, could also contribute to the observed decline in stratospheric NO2 above Jungfraujoch.

Citation: Hendrick, F., Mahieu, E., Bodeker, G. E., Boersma, K. F., Chipperfield, M. P., De Mazière, M., De Smedt, I., Demoulin, P., Fayt, C., Hermans, C., Kreher, K., Lejeune, B., Pinardi, G., Servais, C., Stübi, R., van der A, R., Vernier, J.-P., and Van Roozendael, M.: Analysis of stratospheric NO2 trends above Jungfraujoch using ground-based UV-visible, FTIR, and satellite nadir observations, Atmos. Chem. Phys., 12, 8851-8864, doi:10.5194/acp-12-8851-2012, 2012.
 
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