Size-dependent surface free energy and tolman-corrected droplet nucleation of TIP4P/2005 water

Mark N. Joswiak, Nathan Duff, Michael F. Doherty, Baron Peters

Research output: Contribution to journalArticlepeer-review

Abstract

Classical nucleation theory is notoriously inaccurate when using the macroscopic surface free energy for a planar interface. We examine the size dependence of the surface free energy for TIP4P/2005 water nanodroplets (radii ranging from 0.7 to 1.6 nm) at 300 K with the mitosis method, that is, by reversibly splitting the droplets into two subclusters. We calculate the Tolman length to be -0.56 ± 0.09 Å, which indicates that the surface free energy of water droplets that we investigated is 5-11 mJ/m2 greater than the planar surface free energy. We incorporate the computed Tolman length into a modified classical nucleation theory (δ-CNT) and obtain modified expressions for the critical nucleus size and barrier height. δ-CNT leads to excellent agreement with independently measured nucleation kinetics.

Original languageEnglish (US)
Pages (from-to)4267-4272
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume4
Issue number24
DOIs
StatePublished - Dec 19 2013
Externally publishedYes

Keywords

  • classical nucleation theory
  • curvature
  • hybrid Monte Carlo
  • mitosis method
  • surface tension

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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