The rate at which ozone is increasing in the troposphere is uncertain due to the lack of accurate long‐term measurements. Old ozone measurements obtained at the Pic du Midi Observatory (3000 m high, southwestern France) were recently rediscovered. Four sets of data available at this station are presented herein: (1) 1874–1881 and (2) 1881–1909 by the Schönbein method and (3) 1982–1984 and (4) 1990–1993 by UV absorption analyzers. The results show an increase in ozone by a factor of 5 since the beginning of the twentieth century, corresponding to an exponential increase of 1.6% per year, although this trend is probably higher (2.4% per year) for the last few decades. A stable 10 ppb ozone mixing ratio is observed during the first 20 years of the series, which is representative of the preindustrial era ozone level. The increase is seen to start around 1895. Other data, obtained at various European high‐altitude stations between 1920 and 1980, tie in closely with the Pic du Midi observations. A tentative evaluation of the impact of tropospheric ozone on radiative forcing confirms that ozone is currently the second most significant greenhouse gas, responsible for 22% and 13% of radiative forcing changes since 1800 in the northern and southern hemispheres, respectively. If these rates were to be maintained in the future, ozone would continue to evolve differently in the two hemispheres (maximum level in the northern hemisphere) and could make an even more significant contribution to the radiative forcing of the northern hemisphere.

We present a case study of the decay of a cut-off low over north-west Europe in June 1996, to establish how the stratospheric air initially contained within it was transferred to the troposphere. 'Iko mechanisms for stratosphere-troposphere exchange are examined: direct convective erosion of the base of the low, and filamentation of the outer layers of the low along the flank of the polar jet stream. The approach taken relies on a combination of in-situ ozone and humidity measurements by MOZAIC (Measurement of Ozone and water vapour by Airbus In-service aircraft) aircraft and ozonesondes, and the European Centre for Medium-Range Weather Forecasts analyses. MOZAIC ozone is used to choose two analyses eight days apart at the genesis (14 June 1996) and decay (22 June 1996) of the low which have a consistent ozondpotential-vorticity relationship. Trajectories (both isentropic and three dimensional (3D)) between these two analyses reveal a consistent pattern; at the base of the low (310 K, 450 mb) all the trajectories attain tropospheric PV values whereas, at 320 K, those trajectories that leave the low experience a decrease in PV and those that do not leave the low retain their initial PV. We propose that air parcels leaving the low were stretched into thin filaments along the flank of the jet stream, which made them vulnerable to 3D mixing. A MOZAIC flight on 21 June 1996 provides direct evidence for this process.Up to 22 June 1996 (by which time the low had lost its closed circulation) the satellite images showed very little convection beneath the corresponding PV anomaly. Mixing was only effective at the very base of the stratospheric air at 310 K. On 22 June the remaining remnant of high PV was advected into a region of deep convection over central and eastern Europe, mixing the remaining stratospheric air into the troposphere. Of the initial mass of IOl5 kg of stratospheric air contained in the low, 6 x IOl4 kg was stripped into filaments along the jet and 4 x lOI4 kg remained to be mixed by convection during the period 22-23 June 1996.

Aircraft measurements of ozone, methane, carbon monoxide, relative humidity, and equivalent potential temperature were performed during the TROPOZ II campaign. During the aircraft descent down to Pointe-h-Pitre (16.3øN, 61.5øW), at 2100 UTC on January 12, 1991, two ozone peaks (75 ppb) are observed, one at an altitude of 7.5 km and the other at 3.0 km. A physicochemical interpretation for each ozone peak is proposed in connection with the meteorological context, using radiosounding data, total ozone content from TOMS/NIMBUS 7 and diagnoses issued from analyses by the European Centre for Medium-Range Weather Forecasts, Reading, England. The stratospheric origin of the 7.5-km ozone peak is inferred from negative correlations between ozone and its precursors and from diagnoses based on potential vorticity and ageostrophic circulations depicting the structure of the tropopause fold embedded in the subtropical jet front system. Using an appropriate method to isolate cross-and along-front ageostrophic circulations, we show that much of the observed structure of the tropopause fold can be ascribed to transverse and vertical circulations associated with the irrotational part of the flow. Though the downward extent of the subtropical tropopause fold (400 hPa) is restricted in comparison with typical extratropical tropopause ones (700 hPa), the present results suggest that subtropical tropopause folds may significantly contribute to the global stratosphere-troposphere ozone exchange. The origin of the 3.0-km ozone peak trapped just below the trade wind inversion cannot be ascribed precisely. Analogies with other measurements of dust and aerosols transported over the Atlantic or Pacific in the summer season are discussed. Various possibilities are examined:(1) an earlier stratospheric intrusion event, (2) long-range transport by the trade winds of biomass burning species emitted over West Africa, and (3) fast photochemical ozone formation occurring just below the trade wind inversion within already polluted air parcels originating from remote regions (United States and Gulf of Mexico) after eastward and southward transport around the western Atlantic anticyclone.

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