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Article
Studying vapor-liquid transition using a generalized ensemble
Ames Laboratory Accepted Manuscripts
  • Deepti Ballal, Ames Laboratory
  • Qing Lu, Ames Laboratory
  • Muralikrishna Raju, Iowa State University and Ames Laboratory
  • Xueyu Song, Iowa State University and Ames Laboratory
Publication Date
10-2-2019
Department
Ames Laboratory; Chemistry
OSTI ID+
1568950
Report Number
IS-J 10062
DOI
10.1063/1.5116252
Journal Title
The Journal of Chemical Physics
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)
Citation Information
Deepti Ballal, Qing Lu, Muralikrishna Raju and Xueyu Song. "Studying vapor-liquid transition using a generalized ensemble" Vol. 151 Iss. 13 (2019) p. 134108
Available at: http://works.bepress.com/xueyu-song/58/