Large hemispheric difference in ultrafine aerosol concentrations inthe lowermost stratosphere at mid and high latitudes

2021 
Abstract. The details of aerosol processes and size distributions in the stratosphere are important for both heterogeneous chemistry and aerosol-radiation interactions. Using in-situ, global-scale measurements of the size distribution of particles with diameters > 3 nm from the NASA Atmospheric Tomography Mission (ATom), we identify a mode of ultrafine aerosol in the lowermost stratosphere (LMS) at mid and high latitudes. This mode is substantial only in the northern hemisphere (NH), and was observed in all four seasons. We also observe elevated SO2, an important precursor for new particle formation (NPF) and growth, in the NH LMS. We use box modelling and thermodynamic calculations to show that NPF can occur in the LMS conditions observed on ATom. Aircraft emissions are shown as likely sources of this SO2, as well as a potential source of ultrafine particles directly emitted by, or formed in the plume of the engines. These ultra-fine particles have the potential to grow to larger sizes, and to coagulate with larger aerosol, affecting heterogeneous chemistry and aerosol-radiation interactions. Understanding all sources and characteristics of stratospheric aerosol is important in the context of anthropogenic climate change as well as proposals for climate intervention via stratospheric sulphur injection. This analysis not only adds to the, currently sparse, observations of the global impact of aviation, but also introduces another aspect of climate influence, namely a size distribution shift of the background aerosol distribution in the LMS.
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