Abstract

Abstract Results from the simulation of a coupled chemistry–climate model are presented for the period 1860 to 2005 using the observed greenhouse gas (GHG) and halocarbon concentrations. The model is coupled to a simulated ocean and uniquely includes both detailed tropospheric chemistry and detailed middle atmosphere chemistry, seamlessly from the surface to the model top layer centered at 0.02 hPa. It is found that there are only minor changes in simulated stratospheric temperature and ozone prior to the year 1960. As the halocarbon amounts increase after 1970, the model stratospheric ozone decreases approximately continuously until about 2000. The steadily increasing GHG concentrations cool the stratosphere from the beginning of the twentieth century at a rate that increases with height. During the early period the cooling leads to increased stratospheric ozone. The model results show a strong, albeit temporary, response to volcanic eruptions. While chlorofluorocarbon (CFC) concentrations remain low, the effect of eruptions is shown to increase the amount of HNO3, reducing ozone destruction by the NOx catalytic cycle. In the presence of anthropogenic chlorine, after the eruption of El Chichón and Mt. Pinatubo, chlorine radicals increased and the chlorine reservoirs decreased. The net volcanic effect on nitrogen and chlorine chemistry depends on altitude and, for these two volcanoes, leads to an ozone increase in the middle stratosphere and a decrease in the lower stratosphere. Model lower-stratospheric temperatures are also shown to increase during the last three major volcanic eruptions, by about 0.6 K in the global and annual average, consistent with observations.

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