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  • Title: Inclusion of line tension effect in classical nucleation theory for heterogeneous nucleation: A rigorous thermodynamic formulation and some unique conclusions.
    Author: Singha SK, Das PK, Maiti B.
    Journal: J Chem Phys; 2015 Mar 14; 142(10):104706. PubMed ID: 25770556.
    Abstract:
    A rigorous thermodynamic formulation of the geometric model for heterogeneous nucleation including line tension effect is missing till date due to the associated mathematical hurdles. In this work, we develop a novel thermodynamic formulation based on Classical Nucleation Theory (CNT), which is supposed to illustrate a systematic and a more plausible analysis for the heterogeneous nucleation on a planar surface including the line tension effect. The appreciable range of the critical microscopic contact angle (θc), obtained from the generalized Young's equation and the stability analysis, is θ∞ < θc < θ' for positive line tension and is θM < θc < θ∞ for negative line tension. θ∞ is the macroscopic contact angle, θ' is the contact angle for which the Helmholtz free energy has the minimum value for the positive line tension, and θM is the local minima of the nondimensional line tension effect for the negative line tension. The shape factor f, which is basically the dimensionless critical free energy barrier, becomes higher for lower values of θ∞ and higher values of θc for positive line tension. The combined effect due to the presence of the triple line and the interfacial areas (f(L) + f(S)) in shape factor is always within (0, 3.2), resulting f in the range of (0, 1.7) for positive line tension. A formerly presumed appreciable range for θc(0 < θc < θ∞) is found not to be true when the effect of negative line tension is considered for CNT. Estimation based on the property values of some real fluids confirms the relevance of the present analysis.
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