1National Institute of Water and Atmospheric Research, Christchurch, New Zealand
2Department of Chemistry, University of Canterbury, New Zealand
3Bodeker Scientific, Alexandra, New Zealand
4Physical-Meteorological Observatory Davos/World Radiation Center, Davos, Switzerland
5Institute for Atmospheric and Climate Science ETH, Zurich, Switzerland
Abstract. Through the 21st century, anthropogenic emissions of the greenhouse gases N2O and CH4 are projected to increase, thus increasing their atmospheric concentrations. Consequently, reactive nitrogen species produced from N2O and reactive hydrogen species produced from CH4 are expected to play an increasingly important role in determining stratospheric ozone concentrations. Eight chemistry-climate model simulations were performed to assess the sensitivity of stratospheric ozone to different emissions scenarios for N2O and CH4. Global-mean total column ozone increases through the 21st century in all eight simulations as a result of CO2-induced stratospheric cooling and decreasing stratospheric halogen concentrations. Larger N2O concentrations were associated with smaller ozone increases, due to reactive nitrogen-mediated ozone destruction. In the simulation with the largest N2O increase, global-mean total column ozone increased by 4.3 DU through the 21st century, compared with 10.0 DU in the simulation with the smallest N2O increase. In contrast, larger CH4 concentrations were associated with larger ozone increases; global-mean total column ozone increased by 16.7 DU through the 21st century in the simulation with the largest CH4 concentrations and by 4.4 DU in the simulation with the lowest CH4 concentrations. CH4 leads to ozone loss in the upper and lower stratosphere by increasing the rate of reactive hydrogen-mediated ozone loss cycles, however in the lower stratosphere and troposphere, CH4 leads to ozone increases due to photochemical smog-type chemistry. In addition to this mechanism, total column ozone increases due to H2O-induced cooling of the stratosphere, and slowing of the chlorine-catalyzed ozone loss cycles due to an increased rate of the CH4 + Cl reaction. Stratospheric column ozone through the 21st century exhibits a near-linear response to changes in N2O and CH4 surface concentrations, which provides a simple parameterization for the ozone response to changes in these gases.