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International audience; Every year during the Asian summer monsoon season from about mid-June to early September, a stable anticyclonic circulation system forms over the Himalayas. This Asian summer monsoon (ASM) anticyclone has been shown to promote transport of air into the stratosphere from the Asian troposphere, which contains large amounts of anthropogenic pollutants. Essential details of Asian monsoon transport, such as the exact timescales of vertical transport, the role of convection in cross-tropopause exchange, and the main location and level of export from the confined anticyclone to the stratosphere are still not fully resolved. Recent airborne observations from campaigns near the ASM anticyclone edge and centre in 2016 and 2017, respectively, show a steady decrease in carbon monoxide (CO) and increase in ozone (O3) with height starting from tropospheric values of around 100 ppb CO and 30 50 ppb O3 at about 365 K potential temperature. CO mixing ratios reach stratospheric background values below ∼ 25 ppb at about 420 K and do not show a significant vertical gradient at higher levels, while ozone continues to increase throughout the altitude range of the aircraft measurements. Nitrous oxide (N2O) remains at or only marginally below its 2017 tropospheric mixing ratio of 333 ppb up to about 400 K, which is above the local tropopause. A decline in N2O mixing ratios that indicates a significant contribution of stratospheric air is only visible above this level. Based on our observations, we draw the following picture of vertical transport and confinement in the ASM anticyclone: rapid convective uplift transports air to near 16 km in altitude, corresponding to potential temperatures up to about 370 K. Although this main convective outflow layer extends above the level of zero radiative heating (LZRH), our observations of CO concentration show little to no evidence of convection actually penetrating the tropopause. Rather, further ascent occurs more slowly, consistent with isentropic vertical velocities of 0.7 1.5 K d-1. For the key tracers (CO, O3, and N2O) in our study, none of which are subject to microphysical processes, neither the lapse rate tropopause (LRT) around 380 K nor the cold point tropopause (CPT) around 390 K marks a strong discontinuity in their profiles. Up to about 20 to 35 K above the LRT, isolation of air inside the ASM anticyclone prevents significant in-mixing of stratospheric air (throughout this text, the term in-mixing refers specifically to mixing processes that introduce stratospheric air into the predominantly tropospheric inner anticyclone). The observed changes in CO and O3 likely result from in situ chemical processing. Above about 420 K, mixing processes become more significant and the air inside the anticyclone is exported vertically and horizontally into the surrounding stratosphere.

Measurements of ozone vertical profiles are valuable for the evaluation of atmospheric chemistry models and contribute to the understanding of the processes controlling the distribution of tropospheric ozone. The longest record of ozone vertical profiles is provided by ozone sondes, which have a typical frequency of 4 to 12 profiles a month. Here we quantify the uncertainty introduced by low frequency sampling in the determination of means and trends. To do this, the high frequency MOZAIC (Measurements of OZone, water vapor, carbon monoxide and nitrogen oxides by in-service AIrbus airCraft) profiles over airports, such as Frankfurt, have been subsampled at two typical ozone sonde frequencies of 4 and 12 profiles per month. We found the lowest sampling uncertainty on seasonal means at 700 hPa over Frankfurt, with around 5% for a frequency of 12 profiles per month and 10% for a 4 profile-a-month frequency. However the uncertainty can reach up to 15 and 29% at the lowest altitude levels. As a consequence, the sampling uncertainty at the lowest frequency could be higher than the typical 10% accuracy of the ozone sondes and should be carefully considered for observation comparison and model evaluation. We found that the 95% confidence limit on the seasonal mean derived from the subsample created is similar to the sampling uncertainty and suggest to use it as an estimate of the sampling uncertainty. Similar results are found at six other Northern Hemisphere sites. We show that the sampling substantially impacts on the inter-annual variability and the trend derived over the period 1998–2008 both in magnitude and in sign throughout the troposphere. Also, a tropical case is discussed using the MOZAIC profiles taken over Windhoek, Namibia between 2005 and 2008. For this site, we found that the sampling uncertainty in the free troposphere is around 8 and 12% at 12 and 4 profiles a month respectively.

An ozone climatology based on ozone soundings for the last 15 years has been constructed for model evaluation and comparisons to other observations. Vertical ozone profiles for 41 stations around the globe have been compiled and averaged for the years 1980–1994 and 1995–2009. The climatology provides information about the median and the width of the ozone probability distribution function, as well as interannual variability of ozone between 1995 and 2009, in pressure and tropopause-referenced altitudes. In addition to single stations, regional aggregates are presented, combining stations with similar ozone characteristics. The Hellinger distance is introduced as a new diagnostic to compare the variability of ozone distributions within each region and used for model evaluation purposes. This measure compares not only the mean, but also the shape of distributions. The representativeness of regional aggregates is discussed using independent observations from surface stations and MOZAIC aircraft data. Ozone from all of these data sets show an excellent agreement within the range of the interannual variability, especially if a sufficient number of measurements are available, as is the case for West Europe. Within the climatology, a significant longitudinal variability of ozone in the troposphere and lower stratosphere in the northern mid- and high latitudes is found. The climatology is used to evaluate results from two model intercomparison activities, HTAP for the troposphere and CCMVal2 for the tropopause region and the stratosphere. HTAP ozone is in good agreement with observations in the troposphere within their range of uncertainty, but ozone peaks too early in the Northern Hemisphere spring. The strong gradients of ozone around the tropopause are less well captured by many models. Lower stratospheric ozone is overestimated for all regions by the multi-model mean of CCMVal2 models. Individual models also show major shortcomings in reproducing the shape of ozone probability distribution functions in various regions and different altitudes, which might have significant implications for the radiative budgets in those models.

Chemical ozone loss in winter 1991–1992 is recalculated based on observations of the HALOE satellite instrument, Version 19, ER-2 aircraft measurements and balloon data. HALOE satellite observations are shown to be reliable in the lower stratosphere below 400 K, at altitudes where the measurements are most likely disturbed by the enhanced sulfate aerosol loading, as a result of the Mt.~Pinatubo eruption in June 1991. Significant chemical ozone loss (13–17 DU) is observed below 380 K from Kiruna balloon observations and HALOE satellite data between December 1991 and March 1992. For the two winters after the Mt. Pinatubo eruption, HALOE satellite observations show a stronger extent of chemical ozone loss towards lower altitudes compared to other Arctic winters between 1991 and 2003. In spite of already occurring deactivation of chlorine in March 1992, MIPAS-B and LPMA balloon observations indicate that chlorine was still activated at lower altitudes, consistent with observed chemical ozone loss occurring between February and March and April. Large chemical ozone loss of more than 70 DU in the Arctic winter 1991–1992 as calculated in earlier studies is corroborated here.