Size-dependent stratospheric droplet composition in Lee wave temperature fluctuations and their potential role in PSC freezing

Rapid temperature fluctuations are shown to cause liquid H2SO4/HNO3/H2O stratospheric aerosols to depart considerably from thermodynamic equilibrium. While HNO3 uptake by larger droplets is diffusively hindered, small droplets can approach the composition of a pure binary HNO3/H2O solution with up to 52 wt% HNO3, 48 wt% H2O and very small amounts of H2SO4. The stoichiometry of these droplets is close to that of nitric acid trihydrate (NAT) and freezing experiments suggest that this could be a suitable pathway for the formation of frozen polar stratospheric clouds (PSCs) of type‐Ia.