A Holistic Description of Immersion Freezing of Water and Aqueous Solution Droplets Using a Water Activity Based Model
Abstract
Immersion freezing of water and aqueous solutions by particles acting as ice nuclei (IN) is a common process of heterogeneous ice nucleation in the atmosphere where it results in the glaciation of mixed-phase and cirrus clouds. Using a variety of IN types suspended in various aqueous solutions and pure water, we find that immersion freezing temperatures and kinetics can be described solely by temperature, T, and solution water activity, aw, which is the ratio of the vapor pressure of the solution and the saturation water vapor pressure under the same conditions and, in equilibrium, is equivalent to relative humidity (RH). This allows the freezing point and corresponding heterogeneous ice nucleation rate coefficient, Jhet, to be uniquely expressed by T and aw, a result termed the aw based immersion freezing model (ABIFM). This method is independent of the nature of the solute, applicable for pure water droplet freezing which is significant for mixed-phase cloud formation, and accounts for several varying parameters, including cooling rate and IN surface area, while providing a holistic description of immersion freezing capable of predicting of freezing temperatures, Jhet, frozen fractions, ice particle production rates and numbers. Our findings are based on experimental freezing data collected for various IN surface areas and cooling rates of droplets containing marine biogenic material, two soil humic acids, four mineral dusts, and one organic monolayer acting as IN. For all investigated IN types we demonstrate that droplet freezing temperatures increase as IN surface area increases. Similarly, droplet freezing temperatures increase as the cooling rate decreases. The experimental data implicitly questions the common notion that one active site initiates the formation of an ice embryo leading to the crystallization of the aqueous phase. The log10(Jhet) values for the various IN types derived exclusively by T and aw, provide a complete description of the heterogeneous ice nucleation kinetics. Thus, the ABIFM can be applied over the entire range of T, RH, total IN surface area, and cloud activation timescales typical of atmospheric conditions. Lastly, we demonstrate that ABIFM can be used to derive frozen fractions of droplets and ice particle production for atmospheric models of cirrus and mixed phase cloud conditions.
- Publication:
-
AGU Fall Meeting Abstracts
- Pub Date:
- December 2013
- Bibcode:
- 2013AGUFM.A31J..08K
- Keywords:
-
- 0305 ATMOSPHERIC COMPOSITION AND STRUCTURE Aerosols and particles;
- 0320 ATMOSPHERIC COMPOSITION AND STRUCTURE Cloud physics and chemistry;
- 3311 ATMOSPHERIC PROCESSES Clouds and aerosols