Argon nucleation in a cryogenic supersonic nozzle

We have measured pressures p and temperatures T corresponding to the maximum nucleation rate of argon in a cryogenic supersonic nozzle apparatus where the estimated nucleation rates are J=10(17+/-1) cm(-3) s(-1). As T increases from 34 to 53 K, p increases from 0.47 to 8 kPa. Under these conditions, classical nucleation theory predicts nucleation rates of 11-13 orders of magnitude lower than the observed rates while mean field kinetic nucleation theory predicts the observed rates within 1 order of magnitude. The current data set appears consistent with the measurements of Iland et al. [J. Chem. Phys. 127, 154506 (2007)] in the cryogenic nucleation pulse chamber. Combining the two data sets suggests that classical nucleation theory fails because it overestimates both the critical cluster size and the excess internal energy of the critical clusters.