The Relationship of Loss, Mean Age of Air and the Distribution of CFC's to Stratospheric Circulation and Implications for Atmospheric Lifetimes

Model-derived estimates of the annually integrated destruction and lifetime for various ozone depleting substances (ODSs) depend on the simulated stratospheric transport and mixing in the global model used to produce the estimate. Observations in the middle and high latitude lower stratosphere show that the mean age of an air parcel (i.e., the time since its stratospheric entry) is related to the fractional release for the ODs (i.e., the amount of the ODS that has been destroyed relative to the amount at the time of stratospheric entry). We use back trajectory calculations to produce an age spectrum, and explain the relationship between the mean age and the fractional release by showing that older elements in the age spectrum have experienced higher altitudes and greater ODs destruction than younger elements. In our study, models with faster circulations produce distributions for the age-of-air that are 'young' compared to a distribution derived from observations. These models also fail to reproduce the observed relationship between the mean age of air and the fractional release. Models with slower circulations produce both realistic distributions for mean age and a realistic relationship between mean age and fractional release. These models also produce a CFCl3 lifetime of approximately 56 years, longer than the 45 year lifetime used to project future mixing ratios. We find that the use of flux boundary conditions in assessment models would have several advantages, including consistency between ODS evolution and simulated loss even if the simulated residual circulation changes due to climate change.