On the probability of nucleation at the surface of freezing drops.
Recent publications have proposed that nucleation in the freezing of supercooled drops occurs at the drop surface, an idea supported by statistical thermodynamic arguments by Cahn [J. Chem. Phys. 1977, 66, 3667] coupled with thermodynamic arguments by Tabazadeh et al. [Proc. Natl. Acad. Sci. U.S.A. 2002, 99, 15873]. Whether this phenomenon is general is examined by molecular dynamics simulations of the freezing of deeply supercooled liquid clusters of SeF6. It is found for this model system that while nucleation occurs not infrequently at the surface, it more often takes place in the interior. The probability for surface nucleation increases with the depth of supercooling. How this relates to theories of Cahn and Tabazadeh et al. is discussed briefly.
Turner
Giles W
GW
Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, USA.
Bartell
Lawrence S
LS