ALBERT

Description: Ozonesonde records from the early 1990's through 2008 over two subtropical stations, Irene (near Pretoria, South Africa) and Réunion Island (21° S, 55° W, ~3500 km NE of Irene in the Indian Ocean) were reported to exhibit free tropospheric (FT) ozone increases. Over Irene a large increase in the urban-influenced boundary layer (BL, 1.5–4 km) was also observed during the 18 year period, equivalent to 30% decade−1. Here we show that the Irene BL trend is at least partly due to a gradual change in the sonde launch times from early morning to the midday period. The FT ozone profiles over Irene in 1990–2007 are re-examined, filling in a 1995–1999 gap with ozone profiles taken by Measurements of Ozone by Airbus In-service Aircraft (MOZAIC) over nearby Johannesburg. A multivariate regression model that accounts for the annual ozone cycle, ENSO and possible tropopause changes was applied to monthly averaged Irene data from 4–11 km and to 1992–2011 Réunion sonde data from 4–15 km. Statistically significant trends appear predominantly in the middle and upper troposphere (UT, 4–11 km over Irene, 5–13 km over Réunion) in winter (June–August), with increases ~1 ppbv yr−1 over Irene and ~2 ppbv yr−1 over Réunion. These changes are equivalent to ~25% and 40–50% decade−1, respectively. Both stations also display smaller positive trends in summer with a 50% decade−1 ozone increase near the tropopause over Réunion in December. To explain the ozone increases, we investigated a time series of dynamical markers, e.g., potential vorticity (PV) at 330–350 K. PV affects UT ozone over Irene in November–December but displays little relationship to ozone over Réunion. A more likely reason for wintertime FT ozone increases over Irene and Réunion appears to be long-range transport of growing pollution in the Southern Hemisphere. The ozone increases are consistent with trajectory origins of air parcels sampled by the sondes and with recent NOx emissions trends estimated for Africa, South America, and Madagascar. For Réunion trajectories also point to pollution sources from the eastern Indian Ocean.