TY - JOUR

T1 - Self-consistent cluster approach to the homogeneous kinetic nucleation theory

AU - Kalikmanov, V.I.

AU - van Dongen, M.E.H.

PY - 1993/5/1

Y1 - 1993/5/1

N2 - An alternative, self-consistent formulation of the homogeneous nucleation theory has been proposed. This approach differs from the classical Becker-Döring-Zeldovich theory in two respects: (i) evaporation rates are evaluated by referring to the stable equilibrium of a saturated vapor rather than to the constrained metastable equilibrium of a supersaturated vapor; and (ii) for the reference stable equilibrium state the Fisher theory of condensation is used in order to obtain a self-consistent definition of the free-energy barrier for l-cluster formation, where l is the number of molecules in the cluster. A comparison of the expressions for the nucleation rate and critical cluster size with the corresponding classical expressions has been made for the different parts of the phase diagram (temperature-supersaturation) and the domain where both theories are close has been found. Predictions of the present theory have been compared with the experimental results on nucleation of n-nonane for the three sets of experiments (diffusion cloud chamber, fast-expansion cloud chamber, and two-piston cloud chamber). It has been shown that the present theory has a much better agreement with experimental results for n-nonane than the classical theory.

AB - An alternative, self-consistent formulation of the homogeneous nucleation theory has been proposed. This approach differs from the classical Becker-Döring-Zeldovich theory in two respects: (i) evaporation rates are evaluated by referring to the stable equilibrium of a saturated vapor rather than to the constrained metastable equilibrium of a supersaturated vapor; and (ii) for the reference stable equilibrium state the Fisher theory of condensation is used in order to obtain a self-consistent definition of the free-energy barrier for l-cluster formation, where l is the number of molecules in the cluster. A comparison of the expressions for the nucleation rate and critical cluster size with the corresponding classical expressions has been made for the different parts of the phase diagram (temperature-supersaturation) and the domain where both theories are close has been found. Predictions of the present theory have been compared with the experimental results on nucleation of n-nonane for the three sets of experiments (diffusion cloud chamber, fast-expansion cloud chamber, and two-piston cloud chamber). It has been shown that the present theory has a much better agreement with experimental results for n-nonane than the classical theory.

UR - http://www.scopus.com/inward/record.url?scp=6044224077&partnerID=8YFLogxK

U2 - 10.1103/PhysRevE.47.3532

DO - 10.1103/PhysRevE.47.3532

M3 - Article

AN - SCOPUS:6044224077

VL - 47

SP - 3532

EP - 3539

JO - Physical Review E: Statistical, Physics, Plasmas, Fluids, and Related Interdisciplinary Topics

JF - Physical Review E: Statistical, Physics, Plasmas, Fluids, and Related Interdisciplinary Topics

SN - 1063-651X

IS - 5

ER -