Nonequilibrium coexistence of solid and liquid particles in Arctic stratospheric clouds

Abstract

Observations of polar stratospheric clouds (PSCs) from Ny Ålesund, Spitsbergen, have been examined to quantify the occurrence of solid particles. The polarized backscatter ratio was found to be a more sensitive indicator of the presence of non‐spherical (solid) particles in a PSC than the aerosol depolarization, which approaches zero for clouds containing a large volume of liquid droplets. The analysis corroborates our previous finding that type Ia PSCs cannot be composed of nitric acid trihydrate particles in equilibrium with the gas phase, which would lead to a much too high backscatter ratio. Conversely, type Ib PSCs, previously thought to be composed solely of liquid droplets, often contain a very small fraction of solid particles. These clouds develop a high parallel backscatter, arising from Mie scattering by droplets, and a nonvanishing perpendicular signal due to the few solid particles. Other type Ib PSCs appear to contain only liquid particles. The mixed liquid/solid clouds are observed on the smallest spatial and temporal scale resolvable by the lidar instrument (30 m, l min), implying that their properties are not a result of spatial averaging of different cloud types. Comparison of the observations with optical calculations shows that such nonequilibrium particle distributions are to be expected, as temperature changes are sufficiently rapid to prevent the particles from assuming equilibrium sizes. The observed optical characteristics of type Ia and type Ib clouds can be reproduced in a model by assuming that a very small fraction of the particles are composed of nitric acid hydrate, with the majority being binary H2SO4/H2O or ternary HNO3/H2SO4/H2O droplets.