Argon nucleation in a cryogenic nucleation pulse chamber.

Homogeneous nucleation of argon droplets has been measured with a newly designed cryogenic nucleation pulse chamber presented already in a previous paper [Fladerer and Strey, J. Chem. Phys. 124, 16 (2006)]. Here we present the first systematic nucleation onset data for argon measured in a temperature range from 42 to 58 K and for vapor pressures from 0.3 to 10 kPa. For these data we provide an analytical fit function. From the geometry of the optical detection system and the time of nucleation the experimental nucleation-rate range can be estimated. This allows a comparison of the data with the predictions of classical nucleation theory. We found 16–26 orders of magnitude difference between theory and experiment, and a too strong theoretical dependence of the nucleation rate on temperature. A comparison with the self-consistent theory of Girshick and Chiu [J. Chem. Phys. 93, 1273 (1990)] showed improved temperature dependence but still discrepancies of 11–17 orders of magnitude compared to experimental data. The thermodynamically consistent theory of Kashchiev [J. Chem. Phys. 118, 1837 (2003)] was found to agree rather well with experiment in respect to the temperature dependence and to predict rates about 5-7 orders of magnitude below the experimental ones. With the help of the Gibbs-Thomson equation we were able to evaluate the size of the critical nucleus to be 40–80 argon atoms. [ABSTRACT FROM AUTHOR]