An estimate of the stratospheric contribution to springtime tropospheric ozone maxima using TOPSE measurements and beryllium-7 simulations

Measurements of tropospheric ozone (O3) between 30°N and 70°N show springtime maxima at remote locations. The contribution of seasonal changes in stratosphere–troposphere exchange (STE) to these maxima was investigated using measurements from the Tropospheric Ozone Production about the Spring Equinox Experiment (TOPSE) campaign and the beryllium-7 (7Be) distribution from a calculation driven by fields from the Goddard Earth Observing System Data Assimilation System (GEOS DAS). Comparison with TOPSE measurements revealed that upper tropospheric model-calculated 7Be mixing ratios were reasonable (a change from previous calculations) but that lower tropospheric mixing ratios were too low most likely due to an overestimation of scavenging. Temporal fluctuations were well captured although their amplitudes were often underestimated. Analysis of O3measurements indicated that O3 mixing ratios increased by 5–10% month−1 for θ \u3c 300 K (the underworld) and by 10–15% month−1 for θ \u3e 300 K (the tropospheric middleworld). 7Be mixing ratios decreased with time for θ \u3c 290 K and increased with time for θ \u3e 300 K. Model-calculated middleworld increases of 7Be were a factor of 2 less than measured increases. 7Be with a stratospheric source (strat-7Be) increased by 4.6–8.8% month−1 along TOPSE flight paths within the tropospheric middleworld. Increases in strat-7Be were not seen along TOPSE flight paths in the underworld. Assuming changes in tropospheric O3 with a stratospheric source are the same as changes in strat-7Be and that 50% of O3 in the region of interest is produced in the stratosphere, changes in STE explain 20–60% of O3 increases in the tropospheric middleworld and less than 33% of O3 increases in the underworld