Technical note: Fundamental aspects of ice nucleation via pore condensation and freezing including Laplace pressure and growth into macroscopic ice

Abstract

Pore condensation and freezing (PCF) is an ice nucleation mechanism that explains ice formation at low ice supersaturation. It assumes that liquid water condenses in pores of solid aerosol particles below water saturation, as described by the Kelvin equation, followed by homogeneous ice nucleation when temperatures are below about 235K or immersion freezing at higher temperatures, in case the pores contain active sites that induce ice nucleation. Porewater is under tension (negative pressure) below water saturation as described by the Young-Laplace equation. This negative pressure affects the ice nucleation rates and the stability of the pore ice. Here, pressure-dependent parameterizations of classical nucleation theory are developed to quantify the increase in homogeneous ice nucleation rates as a function of tension and to assess the critical diameter of pores that is required to accommodate ice at negative pressures. Growth of ice out of the pore into a macroscopic ice crystal requires ice supersaturation. This supersaturation as a function of the pore opening width is derived, assuming that the ice phase first grows as a spherical cap on top of the pore opening before it starts to expand laterally on the particle surface into a macroscopic ice crystal.