Strong Evidence of Heterogeneous Processing on Stratospheric Sulfate
Aerosol in the Extrapolar Southern Hemisphere Following the 2022 Hunga
Tonga-Hunga Ha'apai Eruption
Abstract
The January 2022 eruption of Hunga Tonga-Hunga Ha’apai (HT-HH) caused
the largest enhancement in stratospheric aerosol loading in decades and
produced an unprecedented enhancement in stratospheric water vapor,
which led to strong stratospheric cooling that in turn induced changes
in the large-scale circulation. Here we use satellite measurements of
gas-phase constituents together with aerosol extinction to investigate
the extent to which the thick aerosol, excess moisture, and strong
cooling enabled heterogeneous chemical processing. In the southern
tropics, unambiguous signatures of substantial chlorine and nitrogen
repartitioning appear over a broad vertical domain almost immediately
after the eruption, with depletion of N2O5, NOx, and HCl accompanied by
enhancement of HNO3, ClO, and ClONO2. After initially rising steeply,
HNO3 and ClO plateau, maintaining fairly constant abundances for several
months. These patterns are consistent with the saturation of N2O5
hydrolysis, suggesting that this reaction is the primary mechanism for
the observed composition changes. The southern midlatitudes and
subtropics show similar but weaker enhancements in ClO and ClONO2. In
those regions, however, effects of anomalous transport dominate the
evolution of HNO3 and HCl, obscuring the signs of heterogeneous
processing. Perturbations in chlorine species are considerably weaker
than those measured in the southern midlatitude stratosphere following
the Australian New Year’s fires in 2020. The moderate HT-HH-induced
enhancements in reactive chlorine seen throughout the southern middle
and low-latitude stratosphere, far smaller than those in typical winter
polar vortices, do not lead to appreciable chemical ozone loss; rather,
extrapolar lower-stratospheric ozone remains primarily controlled by
dynamical processes.