Publication Date

10-2-2019

Department

Ames Laboratory; Chemistry

Campus Units

Ames Laboratory, Chemistry

OSTI ID+

1568950

Report Number

IS-J 10062

DOI

10.1063/1.5116252

Journal Title

The Journal of Chemical Physics

Volume Number

151

Issue Number

13

First Page

134108

Abstract

Homogeneous vapor-liquid nucleation is studied using the generalized Replica Exchange Method (gREM). The generalized ensemble allows the study of unstable states that cannot directly be studied in the canonical ensemble. Along with replica exchange, this allows for efficient sampling of the multiple states in a single simulation. Statistical Temperature Weighted Histogram Analysis Method is used for postprocessing to get a continuous free energy curve from bulk vapor to bulk liquid. gREM allows the study of planar, cylindrical, and spherical interfaces in a single simulation. The excess Gibbs free energy for the formation of a spherical liquid droplet in vapor for a Lennard-Jones system is calculated from the free energy curve and compared against the umbrella sampling results. The nucleation free energy barrier obtained from gREM is then used to calculate the nucleation rate without relying on any classification scheme for separating the vapor and liquid.

DOE Contract Number(s)

AC02-07CH11358

Language

en

Publisher

Iowa State University Digital Repository, Ames IA (United States)

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