Abstract
Abstract. The knowledge of surface ozone mole fractions and their global distribution is of utmost importance due to the impact of ozone on human health and ecosystems and the central role of ozone in controlling the oxidation capacity of the troposphere. The availability of long-term ozone records is far better in the Northern than in the Southern Hemisphere, and recent analyses of the seven accessible records in the Southern Hemisphere have shown inconclusive trends. Since late 1995, surface ozone is measured in situ at "El Tololo", a high-altitude (2200 m a.s.l.) and pristine station in Chile (30° S, 71° W). The dataset has been recently fully quality controlled and reprocessed. This study presents the observed ozone trends and annual cycles and identifies key processes driving these patterns. From 1995 to 2010, an overall positive trend of ∼ 0.7 ppb decade−1 is found. Strongest trends per season are observed in March and April. Highest mole fractions are observed in late spring (October) and show a strong correlation with ozone transported from the stratosphere down into the troposphere, as simulated with a model. Over the 20 years of observations, the springtime ozone maximum has shifted to earlier times in the year, which, again, is strongly correlated with a temporal shift in the occurrence of the maximum of simulated stratospheric ozone transport at the site. We conclude that background ozone at El Tololo is mainly driven by stratospheric intrusions rather than photochemical production from anthropogenic and biogenic precursors. The major footprint of the sampled air masses is located over the Pacific Ocean. Therefore, due to the negligible influence of local processes, the ozone record also allows studying the influence of El Niño and La Niña episodes on background ozone levels in South America. In agreement with previous studies, we find that, during La Niña conditions, ozone mole fractions reach higher levels than during El Niño conditions.
Highlights
Tropospheric ozone (O3) is a key atmospheric compound that plays an important role in many respects: it acts as a greenhouse gas, which is contributing to radiative forcing of up to 21 % relative to the radiative forcing induced by CO2 (Myhre et al, 2013)
Various processes determine the amount of ozone in the troposphere: ozone is naturally produced by oxidation of methane, by reaction of oxygen with lightning-induced NO production, as well as by photochemical formation in the presence of volatile organic compounds (VOCs), nitrogen
Recent modeling studies postulate that the contribution from stratosphere–troposphere exchange (STE) to the tropospheric ozone burden may be as high as 23 % of the net photochemical production (Stevenson et al, 2006; Sudo and Akimoto, 2007)
Summary
Tropospheric ozone (O3) is a key atmospheric compound that plays an important role in many respects: it acts as a greenhouse gas, which is contributing to radiative forcing of up to 21 % relative to the radiative forcing induced by CO2 (Myhre et al, 2013). Recent modeling studies postulate that the contribution from STE to the tropospheric ozone burden may be as high as 23 % of the net photochemical production (Stevenson et al, 2006; Sudo and Akimoto, 2007). This contribution may change in the future due to climate change and could lead to more than 20 % STE increase (Collins et al, 2003; Hegglin and Shepherd, 2009; Neu et al, 2014)
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