In situ measurements of perturbations to stratospheric aerosol and modeled ozone and radiative impacts following the 2021 La Soufrière eruption

Abstract

Stratospheric aerosols play important roles in Earth's radiative budget and in heterogeneous chemistry. Volcanic eruptions modulate the stratospheric aerosol layer by injecting particles and particle precursors like sulfur dioxide (SO2) into the stratosphere. Beginning on 9 April 2021, La Soufrière erupted, injecting SO2 into the tropical upper troposphere and lower stratosphere, yielding a peak SO2 loading of 0.3–0.4 Tg. The resulting volcanic aerosol plumes dispersed predominately over the Northern Hemisphere (NH), as indicated by the CALIOP/CALIPSO satellite observations and model simulations. From June to August 2021 and May to July 2022, the NASA ER-2 high-altitude aircraft extensively sampled the stratospheric aerosol layer over the continental United States during the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) mission. These in situ aerosol measurements provide detailed insights into the number concentration, size distribution, and spatiotemporal variations of particles within volcanic plumes. Notably, aerosol surface area density and number density in 2021 were enhanced by a factor of 2–4 between 380–500 K potential temperature compared to the 2022 DCOTSS observations, which were minimally influenced by volcanic activity. Within the volcanic plume, the observed aerosol number density exhibited significant meridional and zonal variations, while the mode and shape of aerosol size distributions did not vary. The La Soufrière eruption led to an increase in the number concentration of small particles (<400 nm), resulting in a smaller aerosol effective diameter during the summer of 2021 compared to the baseline conditions in the summer of 2022, as observed in regular ER-2 profiles over Salina, Kansas. A similar reduction in aerosol effective diameter was not observed in ER-2 profiles over Palmdale, California, possibly due to the values that were already smaller in that region during the limited sampling period in 2022. Additionally, we modeled the eruption with the SOCOL-AERv2 aerosol–chemistry–climate model. The modeled aerosol enhancement aligned well with DCOTSS observations, although the direct comparison was complicated by issues related to the model's background aerosol burden. This study indicates that the La Soufrière eruption contributed approximately 0.6 % to Arctic and Antarctic ozone column depletion in both 2021 and 2022, which is well within the range of natural variability. The modeled top-of-atmosphere 1-year global average radiative forcing was −0.08 W m−2 clear-sky and −0.04 W m−2 all-sky. The radiative effects were concentrated in the tropics and NH midlatitudes and diminished to near-baseline levels after 1 year.