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Title: Ab initio calculation of thermodynamic potentials and entropies for superionic water

We construct thermodynamic potentials for two superionic phases of water [with body-centered cubic (bcc) and face-centered cubic (fcc) oxygen lattice] using a combination of density functional theory (DFT) and molecular dynamics simulations (MD). For this purpose, a generic expression for the free energy of warm dense matter is developed and parametrized with equation of state data from the DFT-MD simulations. A second central aspect is the accurate determination of the entropy, which is done using an approximate two-phase method based on the frequency spectra of the nuclear motion. The boundary between the bcc superionic phase and the ices VII and X calculated with thermodynamic potentials from DFT-MD is consistent with that directly derived from the simulations. As a result, differences in the physical properties of the bcc and fcc superionic phases and their impact on interior modeling of water-rich giant planets are discussed.
Authors:
 [1] ;  [2] ;  [1]
  1. Univ. Rostock, Rostock (Germany)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Report Number(s):
SAND-2016-6595J
Journal ID: ISSN 2470-0045; PLEEE8; 644900
Grant/Contract Number:
AC04-94AL85000
Type:
Accepted Manuscript
Journal Name:
Physical Review E
Additional Journal Information:
Journal Volume: 93; Journal Issue: 2; Journal ID: ISSN 2470-0045
Publisher:
American Physical Society (APS)
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
97 MATHEMATICS AND COMPUTING; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
OSTI Identifier:
1263945
Alternate Identifier(s):
OSTI ID: 1239459

French, Martin, Desjarlais, Michael P., and Redmer, Ronald. Ab initio calculation of thermodynamic potentials and entropies for superionic water. United States: N. p., Web. doi:10.1103/PhysRevE.93.022140.
French, Martin, Desjarlais, Michael P., & Redmer, Ronald. Ab initio calculation of thermodynamic potentials and entropies for superionic water. United States. doi:10.1103/PhysRevE.93.022140.
French, Martin, Desjarlais, Michael P., and Redmer, Ronald. 2016. "Ab initio calculation of thermodynamic potentials and entropies for superionic water". United States. doi:10.1103/PhysRevE.93.022140. https://www.osti.gov/servlets/purl/1263945.
@article{osti_1263945,
title = {Ab initio calculation of thermodynamic potentials and entropies for superionic water},
author = {French, Martin and Desjarlais, Michael P. and Redmer, Ronald},
abstractNote = {We construct thermodynamic potentials for two superionic phases of water [with body-centered cubic (bcc) and face-centered cubic (fcc) oxygen lattice] using a combination of density functional theory (DFT) and molecular dynamics simulations (MD). For this purpose, a generic expression for the free energy of warm dense matter is developed and parametrized with equation of state data from the DFT-MD simulations. A second central aspect is the accurate determination of the entropy, which is done using an approximate two-phase method based on the frequency spectra of the nuclear motion. The boundary between the bcc superionic phase and the ices VII and X calculated with thermodynamic potentials from DFT-MD is consistent with that directly derived from the simulations. As a result, differences in the physical properties of the bcc and fcc superionic phases and their impact on interior modeling of water-rich giant planets are discussed.},
doi = {10.1103/PhysRevE.93.022140},
journal = {Physical Review E},
number = 2,
volume = 93,
place = {United States},
year = {2016},
month = {2}
}