Aerosol‐induced chemical perturbations of stratospheric ozone: Three‐dimensional simulations and analysis of mechanisms

Abstract

An atmospheric general circulation model is coupled with a stratospheric photochemical model to simulate the chemical/dynamical perturbations associated with background and volcanically perturbed aerosols in the lower stratosphere. The present work focuses on short‐term anomalies at middle and high latitudes in the northern hemisphere, where large ozone depletions have been observed in late winter and early spring, particularly following the eruption of Mount Pinatubo. Five fully coupled simulations are analyzed, corresponding to a control case with only gas phase chemistry, and cases including heterogeneous chemistry on background aerosols, on El Chichón‐type, and on Pinatubo‐type aerosols. It is found that heterogeneous reactions occurring on sulfate aerosols (background or postvolcanic) can strongly perturb the chemical partitioning in the lower stratosphere, leading to significant ozone depletion through enhanced chlorine, bromine, and odd‐hydrogen catalytic cycles. In the Arctic lower stratosphere, the maximum zonal and March monthly mean local ozone reductions (with respect to the control case) can exceed 15% for the background aerosol case, 40% for the El Chichón case, and 50% for the Pinatubo case. The corresponding zonal mean total column ozone decreases are roughly 5% and 15% for the background and volcanic aerosol cases, respectively. In the most extreme case tested (post‐Pinatubo), a large ozone depletion below 30 mbar is offset to some extent by an ozone increase above that level. The results of a sensitivity study (in which the aerosols are distributed closer to the tropics, as might occur early after an eruption at low latitude) lead to relatively small total ozone depletions at northern high latitudes, and small ozone increases in the tropical lower stratosphere. The reduced impact on total ozone at high latitudes is associated both with local ozone increases above 30 mbar and with poleward transport of enhanced ozone from the tropical lower stratosphere. The ozone increase at low latitudes is the net result of compensating changes in the catalytic destruction cycles involving odd‐nitrogen and chlorine species activated by heterogeneous processes at the low temperatures and abundant sunlight found near the tropical tropopause. Our simulations indicate that ozone variations triggered by volcanic injections of aerosols depend on the global distribution as well as the abundance of the particles and their evolution over time, and on the initial dynamical‐radiative‐chemical state of the atmosphere, which itself exhibits large seasonal and interannual variability.