Atmos. Chem. Phys. Discuss., 9, 1051-1095, 2009
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Global upper-tropospheric formaldehyde: seasonal cycles observed by the ACE-FTS satellite instrument
G. Dufour1, S. Szopa2, M. P. Barkley3, C. D. Boone4, A. Perrin1, P. I. Palmer3, and P. F. Bernath4,5
1Laboratoire Inter-universitaire des Systèmes Atmosphériques (LISA), UMR7583, Universités Paris 12 et Paris 7, CNRS, Créteil, France
2Laboratoire des Sciences du Climat et de l'Environnement (LSCE/IPSL), CNRS-CEA-UVSQ Gif-sur-Yvette, France
3School of GeoSciences, University of Edinburgh, UK
4Department of Chemistry, University of Waterloo, Ontario, N2L 3G1, Canada
5Department of Chemistry, University of York, Heslington, York, YO10 5DD, UK

Abstract. Seasonally-resolved upper tropospheric profiles of formaldehyde (HCHO) observed by the ACE Fourier transform spectrometer (ACE-FTS) on a near-global scale are presented for the time period from March 2004 to November 2006. Large upper tropospheric HCHO mixing ratios (>150 pptv) are observed during the growing season of the terrestrial biosphere in the Northern Hemisphere and during the biomass burning season in the Southern Hemisphere. The total errors estimated for the retrieved mixing ratios range from 30 to 40% in the upper troposphere and increase in the lower stratosphere. The sampled HCHO concentrations are in satisfactory agreement with previous aircraft and satellite observations with a negative bias (<25%) within observation errors. An overview of the seasonal cycle of the upper tropospheric HCHO is given for different latitudes. A maximum is observed during summer, i.e. during the growing season, in the northern mid- and high latitudes. The influence of biomass burning is visible in HCHO upper tropospheric concentrations during the September-to-October period in the southern tropics and subtropics. Comparisons with two state-of-the-art models (GEOS-Chem and LMDz-INCA) show that the models fail to reproduce the seasonal variations observed in the southern tropics and subtropics but they capture well the variations observed in the Northern Hemisphere (correlation >0.9). Both models underestimate the summer maximum over Europe and Russia and differences in the emissions used for North America result in a good reproduction of the summer maximum by GEOS-Chem but in an underestimate by LMDz-INCA. Globally, GEOS-Chem reproduces well the observations on average over one year but has some difficulties in reproducing the spatial variability of the observations. LMDz-INCA shows significant bias in the Southern Hemisphere, likely related to an underestimation of methane, but better reproduces the temporal and spatial variations. The differences between the models underline the large uncertainties that remain in the emissions of HCHO precursors. Observations of the HCHO upper tropospheric profile provided by the ACE-FTS represent a unique data set for investigating and improving our current understanding of the formaldehyde budget and upper tropospheric chemistry.

Citation: Dufour, G., Szopa, S., Barkley, M. P., Boone, C. D., Perrin, A., Palmer, P. I., and Bernath, P. F.: Global upper-tropospheric formaldehyde: seasonal cycles observed by the ACE-FTS satellite instrument, Atmos. Chem. Phys. Discuss., 9, 1051-1095, doi:10.5194/acpd-9-1051-2009, 2009.
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