Large hemispheric difference in nucleation mode aerosol concentrations in the lowermost stratosphere at mid- and high latitudes

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 aerosol smaller than 12 nm 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 nucleation mode particles directly emitted by or formed in the plume of the engines. These nucleation mode 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 aerosols is important in the context of anthropogenic climate change as well as proposals for climate intervention via stratospheric sulfur 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.