Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions

Abstract

Ice clouds in the tropical tropopause layer have a key role in dehydrating air that is entering the stratosphere. Cloud-chamber measurements suggest that their high humidity can be explained if heterogeneous ice nucleation on glassy aerosols is a significant nucleation mechanism in this region. Ice clouds in the tropical tropopause layer play a key role in dehydrating air as it enters the stratosphere1,2. However, in situ measurements show that water vapour within these clouds is unexpectedly supersaturated3,4,5; normally the growth of ice crystals rapidly quenches supersaturation3. The high in-cloud humidity may be related to the low number of ice crystals found in these clouds4,6, but low ice number densities are inconsistent with standard models of cirrus cloud formation involving homogeneous freezing of liquid aerosols7. Aqueous aerosols rich in organic matter are ubiquitous in the atmosphere8,9, and under cirrus conditions they are known to become glassy10,11, that is, amorphous, non-crystalline solids. Here we report experiments in a cloud simulation chamber that demonstrate heterogeneous nucleation of ice on glassy solution droplets. Cirrus residues measured in situ showed ice nuclei rich in oxidized organic matter12, consistent with heterogeneous nucleation on glassy aerosols. In addition, using a one-dimensional cirrus model, we show that nucleation on glassy aerosols may explain low ice crystal numbers and high in-cloud humidity in the tropical tropopause layer. We propose that heterogeneous nucleation on glassy aerosols is an important mechanism for ice nucleation in the tropical tropopause layer.