Combinatorial entropy and phase diagram of partially ordered ice phases

  • MacDowell L
  • Sanz E
  • Vega C
 et al. 
  • 22

    Readers

    Mendeley users who have this article in their library.
  • 44

    Citations

    Citations of this article.

Abstract

A close analytical estimate for the combinatorial entropy of partially ordered ice phases is presented. The expression obtained is very general, as it can be used for any ice phase obeying the Bernal-Fowler rules. The only input required is a number of crystallographic parameters, and the experimentally observed proton site occupancies. For fully disordered phases such as hexagonal ice, it recovers the result deduced by Pauling, while for fully ordered ice it is found to vanish. Although the space groups determined for ice I, VI, and VII require random proton site occupancies, it is found that such random allocation of protons does not necessarily imply random orientational disorder. The theoretical estimate for the combinatorial entropy is employed together with free energy calculations in order to obtain the phase diagram of ice from 0 to 10 GPa. Overall qualitative agreement with experiment is found for the TIP4P model of water. An accurate estimate of the combinatorial entropy is found to play an important role in determining the stability of partially ordered ice phases, such as ice III and ice V.

Get free article suggestions today

Mendeley saves you time finding and organizing research

Sign up here
Already have an account ?Sign in

Find this document

Authors

Cite this document

Choose a citation style from the tabs below

Save time finding and organizing research with Mendeley

Sign up for free