Article (Scientific journals)
On the accuracy of van der Waals inclusive density-functional theory exchange-correlation functionals for ice at ambient and high pressures
Santra, Biswajit; Klimes, Jiri; Tkatchenko, Alexandre et al.
2013In JOURNAL OF CHEMICAL PHYSICS, 139 (15)
Peer reviewed
 

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Abstract :
[en] Density-functional theory (DFT) has been widely used to study water and ice for at least 20 years. However, the reliability of different DFT exchange-correlation (xc) functionals for water remains a matter of considerable debate. This is particularly true in light of the recent development of DFT based methods that account for van der Waals (vdW) dispersion forces. Here, we report a detailed study with several xc functionals (semi-local, hybrid, and vdW inclusive approaches) on ice Ih and six proton ordered phases of ice. Consistent with our previous study [B. Santra, J. Klimes, D. Alfe, A. Tkatchenko, B. Slater, A. Michaelides, R. Car, and M. Scheffler, Phys. Rev. Lett. 107, 185701 (2011)] which showed that vdW forces become increasingly important at high pressures, we find here that all vdW inclusive methods considered improve the relative energies and transition pressures of the high-pressure ice phases compared to those obtained with semi-local or hybrid xc functionals. However, we also find that significant discrepancies between experiment and the vdW inclusive approaches remain in the cohesive properties of the various phases, causing certain phases to be absent from the phase diagram. Therefore, room for improvement in the description of water at ambient and high pressures remains and we suggest that because of the stern test the high pressure ice phases pose they should be used in future benchmark studies of simulation methods for water. (C) 2013 AIP Publishing LLC.
Disciplines :
Physics
Author, co-author :
Santra, Biswajit;  Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany ; Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA
Klimes, Jiri;  Faculty of Physics and Center for Computational Materials Science, University of Vienna, Sensengasse 8/12, A-1090 Wien, Austria
Tkatchenko, Alexandre ;  Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany
Dario, Alfe;  London Centre for Nanotechnology, University College London, London WC1E6BT, United Kingdom ; Department of Physics and Astronomy, University College London, London WC1E6BT, United Kingdom and Department of Earth Sciences, University College London, London WC1E6BT, United Kingdom
Slater, Ben;  Department of Chemistry, University College London, London WC1E6BT, United Kingdom
Michaelides, Angelos;  London Centre for Nanotechnology, University College London, London WC1E6BT, United Kingdom ; Department of Chemistry, University College London, London WC1E6BT, United Kingdom
Car, Roberto;  Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA
Scheffler, Matthias;  Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany
External co-authors :
yes
Title :
On the accuracy of van der Waals inclusive density-functional theory exchange-correlation functionals for ice at ambient and high pressures
Publication date :
2013
Journal title :
JOURNAL OF CHEMICAL PHYSICS
ISSN :
0021-9606
Publisher :
AMER INST PHYSICS, CIRCULATION FULFILLMENT DIV, 2 HUNTINGTON QUADRANGLE, STE 1 N O 1 MELVILLE, NY 11747-4501 USA, Unknown/unspecified
Volume :
139
Issue :
15
Peer reviewed :
Peer reviewed
Commentary :
Article
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