Abstract

Abstract. We present ozone measurements of the Global Atmospheric Sampling Program (GASP) performed from four commercial and one research aircraft in the late 1970s to compare them with respective measurements of the ongoing MOZAIC project. Multi-annual averages of UT/LS ozone were built using the aircraft data sets (1975–1979 and 1994–2001), and long-term changes between the 1970s and 1990s were derived by comparison. The data were binned relative to the dynamical tropopause to separate between UT and LS air masses. LS data were analysed using equivalent latitudes. In the UT, pronounced increases of 20–40% are found over the Middle East and South Asia in the spring and summer seasons. Increases are also found over Japan, Europe, and the eastern parts of the United States depending on season. LS ozone over northern mid- and high latitudes was found to be lower in the 1990s compared to the 1970s in all seasons of the year. In addition, a comparison with long-term changes deduced from ozonesondes is presented. The early 1970s European Brewer-Mast (BM) sonde data agree with GASP within the range of uncertainty (UT) or measured slightly less ozone (LS). In contrast, the 1990s BM sensors show consistently and significantly higher UT/LS ozone values than MOZAIC. This unequal behaviour of aircraft/sonde comparisons in the 1970s and 1990s leads to differences in the estimated long-term changes over Europe: while the comparison between GASP and MOZAIC indicates ozone changes of −5% to 10% over Europe, the sondes suggest a much larger increase of 10%–35% depending on station and season, although statistical significance is not conclusive due to data sample limitations. In contrast to the BM sondes, the Electrochemical Cell (ECC) sonde at Wallops Island, USA, measured higher UT ozone than both GASP and MOZAIC. Hence, long-term changes from GASP/MOZAIC agree within the range of uncertainty with the changes deduced from Wallops Island.

Highlights

  • The upper troposphere and lower stratosphere (UT/less ozone (LS)) constitute regions of major concern for both climate impact and the surface environment

  • We present upper troposphere and lower stratosphere (UT/LS) ozone changes derived from the comparison between Global Atmospheric Sampling Program (GASP) and MOZAIC data

  • Changes of UT/LS ozone between the late 1970s and the second half of the 1990s deduced from the GASP and MOZAIC data sets are described separately for the UT (Sect. 3.1) and the LS (Sect. 3.2)

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Summary

Introduction

The upper troposphere and lower stratosphere (UT/LS) constitute regions of major concern for both climate impact and the surface environment. Because of the radiative properties and temperature structure of the atmosphere, changes in ozone have their largest impact on climate when they occur in the UT/LS (Forster and Shine, 1997). UT/LS ozone is determined by both transport and chemistry depending on region and season of the year. The relative contributions of different processes are expected to vary strongly across the tropopause. At these altitudes, ozone is produced from precursor substances including nitrogen oxides (NOx), volatile organic compounds (VOCs), and carbon monoxide (CO) under the influence of sunlight and destroyed mainly in reactions with HOx radicals (e.g., Rohrer, 1995).

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