Abstract

Abstract. This paper evaluates the agreement between stratospheric NO2 retrievals from infrared limb sounders (Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and High Resolution Dynamics Limb Sounder (HIRDLS)) and solar UV/VIS backscatter sensors (Ozone Monitoring Instrument (OMI), Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY) limb and nadir) over the 2005–2007 period and across the seasons. The observational agreement is contrasted with the representation of NO2 profiles in 3-D chemical transport models such as the Whole Atmosphere Community Climate Model (WACCM) and TM4. A conclusion central to this work is that the definition of a reference for stratospheric NO2 columns formed by consistent agreement among SCIAMACHY, MIPAS and HIRDLS limb records (all of which agree to within 0.25 × 1015 molecules cm−2 or better than 10%) allows us to draw attention to relative errors in other data sets, e.g., (1) WACCM overestimates NO2 densities in the extratropical lower stratosphere, particularly in the springtime and over northern latitudes by up to 35% relative to limb observations, and (2) there are remarkable discrepancies between stratospheric NO2 column estimates from limb and nadir techniques, with a characteristic seasonally and latitudinally dependent pattern. We find that SCIAMACHY nadir and OMI stratospheric columns show overall biases of −0.5 × 1015 molecules cm−2 (−20%) and +0.6 × 1015 molecules cm−2 (+20%) relative to limb observations, respectively. It is argued that additive biases in nadir stratospheric columns are not expected to affect tropospheric retrievals significantly, and that they can be attributed to errors in the total slant column density, related either to algorithmic or instrumental effects. In order to obtain accurate and long-term time series of stratospheric NO2, an effort towards the harmonization of currently used differential optical absorption spectroscopy (DOAS) approaches to nadir retrievals becomes essential, as well as their agreement to limb and ground-based observations, particularly now that limb techniques are giving way to nadir observations as the next generation of climate and air quality monitoring instruments pushes forth.

Highlights

  • Nitrogen dioxide (NO2) is a major air pollutant in the troposphere produced mainly from fossil fuel burning, and from biomass burning, microbial soil activity and lightning (Lamarque, 1996)

  • The mean relative difference (MRD) between two records is calculated by dividing the mean absolute difference by the mean profile, which gives an indication of bias whenever larger than the combined precisions of the two records – which is on the order of 1–2 %, given the large number of profiles included in the difference

  • The agreement between High Resolution Dynamics Limb Sounder (HIRDLS) and SCIAMACHY limb profiles is confirmed within 20 % over extratropical latitudes, excluding the late summer (JJA) and early fall (SON) season over the Southern Hemisphere, where HIRDLS is affected by a positive bias of about 60 % at and below peak NO2 levels

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Summary

Introduction

Nitrogen dioxide (NO2) is a major air pollutant in the troposphere produced mainly from fossil fuel burning, and from biomass burning, microbial soil activity and lightning (Lamarque, 1996). NO2 is a major ozonedepleting substance produced primarily from the oxidation of nitrous oxide (N2O), which in turn arises from biogenic sources in soils, oceans and cultivated areas. Denitrification, or the removal of stratospheric NO2 through formation and deposition of polar stratospheric ice particles, is a key microphysical process in the formation of polar ozone holes (Farman et al, 1985). The representation of denitrification remains unrealistic in current chemical transport models (CTMs) during cold winters (WMO, 2003). For long-term trend studies, stratospheric NO2 remains

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