Ab-initio density-functional lattice-dynamics studies of ice

Côté, AS; Morrison, I; Cui, XY; Jenkins, S; Ross, DK

Abstract

We present the results of first-principles computational studies of the dynamical properties of hexagonal ice using both the ab-initio pseudopotential method and the full-potential augmented plane-wave method. Properties obtained using both the generalized gradient approximation (GGA) and the meta-GGA in density-functional theory are compared. The lattice-dynamical properties of the structures are obtained using a finite-difference evaluation of the dynamical matrix and force-constant matrix from atomic forces. Phonon dispersion is evaluated by the direct determination of the force-constant matrix in supercells derived from the primitive molecule unit cells with the assumption that force constants are zero beyond the second molecular nearest neighbors. The k-dependent phonon frequencies are then obtained from the force-constant matrix and dispersion relations, and the Brillouin-zone integrated density of states is evaluated. The importance of phonon dispersion in the various regions of the phonon spectra is then assessed and compared to existing neutron-scattering data. Frozen-phonon calculations are used to compare phonon frequencies evaluated in both the GGA and meta-GGA.

Citation

Côté, A., Morrison, I., Cui, X., Jenkins, S., & Ross, D. (2003). Ab-initio density-functional lattice-dynamics studies of ice. Canadian Journal of Physics, 81(1-2), 115-122. https://doi.org/10.1139/p03-003

• Journal Article Type: Article
• Publication Date: Jan 1, 2003
• Deposit Date: Aug 23, 2007
• Publicly Available Date: Aug 23, 2007
• Journal: Canadian Journal of Physics
• Print ISSN: 0008-4204
• Publisher: NRC Research Press
• Peer Reviewed: Peer Reviewed
• Volume: 81
• Issue: 1-2
• Pages: 115-122
• DOI: https://doi.org/10.1139/p03-003
• Publisher URL: http://dx.doi.org/10.1139/p03-003
• Related Public URLs: http://www.nrc-cnrc.gc.ca/; http://pubs.nrc-cnrc.gc.ca/rp-ps/journalDetail.jsp?jcode=cjp&lang=eng