Microphysical modeling of the 1999-2000 Arctic winter 2. Chlorine activation and ozone depletion

Abstract

The effect of polar stratospheric clouds (PSCs) on ozone depletion during the 1999-2000 Arctic winter has been assessed using a coupled microphysical/photochemical model. Scenarios spanned a large range of denitrification levels, with up to 80% vortex-averaged denitrification and localized dehydration. PSC composition was varied, exploring sensitivity to heterogeneous reaction rates. PSC formation during February was critical in causing severe ozone depletion below 500 K. Heterogeneous chemistry on these PSCs was able to continuously reactivate the newly produced ClONO2. Only 30-40% vortex-averaged ozone loss would have occurred without this chlorine reactivation; with it, 21-32% more ozone loss is possible. During February (unlike earlier in the winter), chlorine reactivation and ozone loss were sensitive to heterogeneous chemistry: varying the reactivities altered ozone loss by 11%. An analysis of the critical temperatures for heterogeneous chemistry demonstrates the importance of temperatures near the nitric acid trihydrate condensation point, where many uncertainties influence heterogeneous reaction rates. Chlorine reactivation during February also prevented denitrification from enhancing ozone loss until March: 70% vortex-averaged denitrification only enhanced ozone depletion by 3% on 10 March. The mid-March vortex breakup probably limited the extent of ozone depletion; if the vortex had remained stable until 15 April, 16% ozone loss (out of a total 68% ozone loss) could be caused by 70% denitrification. Ozone loss intensifies nonlinearly with enhanced denitrification: in individual air parcels with 90% denitrification, 40% ozone loss in mid-April can be attributed to denitrification alone.