High concentrations of ice crystals in upper-tropospheric tropical clouds: is there a link to biomass and fossil fuel combustion?

Eight years of upper-tropospheric (UT) ice crystal measurements with the backscatter cloud probe (BCP), installed on commercial aircraft operated as part of the In-Service Aircraft for a Global Observing System (IAGOS), have been analyzed to assess the frequency and characteristics of extreme ice crystal events (EIEs), defined in this study as encounters with clouds that have number concentrations exceeding 5000 L-1. A total of 3196 events, in clouds of horizontal extent >= 2.5 km, were identified during the period from December 2011 to March 2020 in the latitude band between 30 degrees S and 30 degrees N. Regions of anthropogenic sources of carbon monoxide, with particles that can alter cloud microphysics, were attributed to these EIEs in UT clouds using the SOFT-IO model. The evaluation of low- and upper-level kinematic variables from the European Centre for Medium-Range Weather Forecasts (ERA5) reanalysis, combined with spatial distributions of aerosol optical depth and regions of biomass burning, highlights the physical mechanisms by which the particles are lofted to flight levels in regions of deep convection. The maps of lightning frequency, derived from the World Wide Lightning Location Network (WWLLN), provide additional evidence of the role of deep convection in transporting aerosol particles, cloud hydrometeors and carbon monoxide to aircraft cruising altitudes. The evaluation of aerosol particle mass concentrations and composition from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) contributes additional evidence for a link between regions of EIEs and surface emissions of dust, black carbon (BC), organic carbon (OC) and sulfate particles. Given the composition of the source aerosols and the role of deep convection in their transport to the UT, the sampled ice clouds likely originate from the homogeneous or heterogeneous freezing of droplets formed on these particles, as has been reported in previous studies. The results from this study, which have been obtained from a large sample of measurements, have ramifications related to satellite measurement validation, weather forecasting and climate change. In addition, over 2000 of the randomly sampled clouds had derived ice water contents larger than 1 gm(-3), a concentration that is considered potentially hazardous to commercial aircraft operations.