Abstract. Our quantitative understanding of natural tropospheric
ozone concentrations is limited by the paucity of reliable measurements
before the 1980s. We utilize the existing measurements to compare the
long-term ozone changes that occurred within the marine boundary layer at
northern and southern midlatitudes. Since 1950 ozone concentrations have
increased by a factor of 2.1 ± 0.2 in the Northern Hemisphere (NH) and
are presently larger than in the Southern Hemisphere (SH), where only a much
smaller increase has occurred. These changes are attributed to increased
ozone production driven by anthropogenic emissions of photochemical ozone
precursors that increased with industrial development. The greater ozone
concentrations and increases in the NH are consistent with the predominant
location of anthropogenic emission sources in that hemisphere. The available
measurements indicate that this interhemispheric gradient was much smaller
and was likely reversed in the pre-industrial troposphere with higher
concentrations in the SH. Six Earth system model (ESM) simulations indicate
similar total NH increases (1.9 with a standard deviation of 0.3), but they
occurred more slowly over a longer time period, and the ESMs do not find
higher pre-industrial ozone in the SH. Several uncertainties in the ESMs may
cause these model–measurement disagreements: the assumed natural nitrogen
oxide emissions may be too large, the relatively greater fraction of ozone
injected by stratosphere–troposphere exchange to the NH may be
overestimated, ozone surface deposition to ocean and land surfaces may not
be accurately simulated, and model treatment of emissions of biogenic
hydrocarbons and their photochemistry may not be adequate.