Proton disorder and elasticity of hexagonal ice and gas hydrates
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This work is devoted to the study of the mechanical properties of hexagonal ice Ih and gas hydrate frameworks sI, sII and sH, taking into account the disorder in the positions of the hydrogen atoms (protons). The article emphasizes the critical role of the elastic energy for the evaluation of the relative energy of the proton configurations. The calculations are performed with the help of the TINKER package using the AMOEBA polarizable force field. The elastic constants, elastic modulus, and anisotropy indices are calculated. It is shown that all gas hydrate frameworks are very isotropic due to their cage-like structure. It was established that one of the reasons for the higher anisotropy of ice Ih is the presence of a large number of highly symmetric proton configurations. The purpose of the article is to overcome the apparent contradiction between the ab initio and force field methods in predicting the relative stability of the proton configurations of ice structures at low temperature. The other purpose is to evaluate the effect of proton disorder on the elastic properties of ice and gas hydrate structures.
KeywordsProton disorder Gas hydrates Hexagonal ice Elastic energy
We thank A.L. Tchougreef for useful discussion. The present work was supported by the Basic Research Program of RAS No. IX.135.2.3.
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Conflict of interest
The authors declare that they have no conflict of interest.
- 1.Petrenko VF, Whitworth RW (1999) Physics of ice. Oxford University Press, OxfordGoogle Scholar
- 18.Fanourgakis GS, Xantheas SS (2008) Development of transferable interaction potentials for water. V. Extension of the flexible, polarizable, Thole-type model potential (TTM3-F, v. 3.0) to describe the vibrational spectra of water clusters and liquid water. J Chem Phys 128:074506CrossRefGoogle Scholar
- 24.Miranda CR, Matsuoka T (2008) First-principles study on mechanical properties of CH4 hydrate. Proceedings of the 6th international conference on gas hydrates (ICGH 2008), 6–10 July 2008, Vancouver, BC, CanadaGoogle Scholar
- 36.Sloan Jr ED (1998) Clathrate hydrates of natural gases, 2nd edn. Dekker, New YorkGoogle Scholar
- 39.Ponder JW (2003) TINKER: software yools for molecular design, 4.1 edn. Washington University School of Medicine, Saint LouisGoogle Scholar
- 41.Leeuw SW, Perram JW, Smith ER (1980) Simulation of electrostatic systems in periodic boundary conditions. I. Lattice sums and dielectric constants. Proc R Soc A 373:27–56Google Scholar
- 42.Frenkel D, Smit B (2002) Understanding molecular simulation: from algorithms to applications, 2nd edn. Academic, San DiegoGoogle Scholar
- 45.Landau LD, Lifshitz EM (1986) Theory of elasticity, vol. 7, 3rd edn. Butterworth-Heinemann, OxfordGoogle Scholar
- 46.Bower AF (2009) Applied mechanics of solids. CRC, Boca RatonGoogle Scholar
- 47.Allen MP, Tildesley DJ (1989) Computer simulation of liquids, 2nd edn. Oxford University Press, OxfordGoogle Scholar
- 49.Nye JF (1985) Physical properties of crystals. Oxford University Press, OxfordGoogle Scholar
- 50.Kittel C (1996) Introduction to solid state physics, 7th edn. Wiley, New YorkGoogle Scholar