On Nucleation Pathways and Particle Size Distribution Evolutions in Stratospheric Aircraft Exhaust Plumes with H₂SO₄ Enhancement

Stratospheric aerosol injection (SAI) is proposed as a means of reducing global warming and climate change impacts. Similar to aerosol enhancements produced by volcanic eruptions, introducing particles into the stratosphere would reflect sunlight and reduce the level of warming. However, uncertainties remain about the roles of nucleation mechanisms, ionized molecules, impurities (unevaporated residuals of injected precursors), and ambient conditions in the generation of SAI particles optimally sized to reflect sunlight. Here, we use a kinetic ion-mediated and homogeneous nucleation model to study the formation of H2SO4 particles in aircraft exhaust plumes with direct injection of H2SO4 vapor. We find that under the conditions that produce particles of desired sizes (diameter similar to 200-300 nm), nucleation occurs in the nascent (t < 0.01 s), hot (T = 360-445 K), and dry (RH = 0.01-0.1%) plume and is predominantly unary. Nucleation on chemiions occurs first, followed by neutral new particle formation, which converts most of the injected H2SO4 vapor to particles. Coagulation in the aging and diluting plumes governs the subsequent evolution to a narrow (sigma(g) = 1.3) particle size distribution. Scavenging by exhaust soot is negligible, but scavenging by acid impurities or incomplete H2SO4 evaporation in the hot exhaust plume and enhanced background aerosols can matter. This research highlights the need to obtain laboratory and/or real-world experiment data to verify the model prediction.