First page Back Continue Last page Text

Notes:


A simple empirical relationship has been found for the homogeneous freezing of aqueous solutions such as sulfuric acid or ammonium sulfate. Lambda is an empirical constant equal to about 1.7.

This figure is also from Koop.

FIGURE 2. Comparison of ice nucleation measurements and models for micron sized aqueous droplets

of (a) H2SO4 and (b) (NH4)2SO4. Diamonds: FTIR experiments;16,17 circles: microscope

experiments;18,19 triangles: emulsion experiments;19-21 squares: electrodynamic balance experiments.22

Dash-dotted line: equilibrium ice melting point curve; dotted line: classical nucleation model for

H2SO4-H2O;23 dashed line: lambda model, see text;25-27 solid line: thermodynamic model, see text.28

The dashed curves indicate results from a model 25-27 in which the freezing

temperature of a solution droplet, Sol

fr T , was calculated according to

, m

2O H

fr

Sol

fr T T T (1)

where H

fr T

2O

is the freezing temperature of a pure water droplet of the same size, m T

is the equilibrium melting point depression of ice in the solution (i.e., Sol

m 273.15-T ),

and is a constant depending on the nature of the solute. The homogenous ice

nucleation rate coefficient in solution, Sol

fr J , is predicted based on the assumption that

), ) 2O H

fr

2O H

fr

Sol

fr

Sol

fr (T J (T J (2)

where ) 2O H

fr

2O H

fr (T J is the homogeneous ice nucleation rate coefficient for pure water,

H

fr J

2O

, at temperature H

fr T

2O

. In the following paragraphs this model will be termed the

“lambda model”. The curves in Figure 2 represent a homogeneous nucleation rate of

J=10 9 cm -3 s -1 and a value of =1.0 for the H2SO4 case, and =1.7 for the (NH4)2SO4

case.27 The formulation of Pruppacher 6 for (T) f J 2O H

fr has been used in these

calculations.

The solid curves indicate the results of a semi-empirical thermodynamic ice

nucleation model which is based on experimental ice freezing data of 18 different

solutes in aqueous solutions.28 This model will be termed the “thermodynamic model”