Issue 19, 2002
From the journal:

Physical Chemistry Chemical Physics

Anharmonicity and guest–host coupling in clathrate hydrates

B. Chazallon,†a   H. Itoh,b   M. Koza,c   W. F. Kuhs*b  and  H. Schober*c  

* Corresponding authors

a Laboratoire de Glaciologie et Géophysique de l'Environnement, 54, rue Molière, Saint-Martin d'Hères Cedex, France

b GZG Abt. Kristallographie, Universität Göttingen, Goldschmidtstr. 1, Göttingen, Germany
E-mail: wkuhs1@gwdg.de

c Institut Laue-Langevin, Grenoble, B. P. 156, Grenoble Cedex, France
E-mail: schober@ill.fr

Abstract

The dynamic response of Ar, Xe, O2 and N2-containing clathrate hydrates has been studied by neutron spectroscopy. Type I and type II clathrate hydrates show some small but significant differences in the low-frequency host contribution to the density of states. Both differ markedly from that of ice Ih and depend only weakly on the guest. While the vibrational modes associated with Xe and Ar are found to be close-to-harmonic, strong temperature dependent shifts are encountered for the O2 and N2 low-frequency vibrations. A coupling of the guest and host vibrations is confirmed by our experiments. Its strength depends strongly on the type of included guest. In particular Xe-hydrate cannot be considered representative as due to the large mass of the guest atom all its vibrational bands fall into the acoustic range of the host lattice.

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Article information

DOI
https://doi.org/10.1039/B202464K
Article type
Paper
Submitted
08 Mar 2002
Accepted
27 Jun 2002
First published
28 Aug 2002

Phys. Chem. Chem. Phys., 2002,4, 4809-4816

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Anharmonicity and guest–host coupling in clathrate hydrates

B. Chazallon, H. Itoh, M. Koza, W. F. Kuhs and H. Schober, Phys. Chem. Chem. Phys., 2002, 4, 4809 DOI: 10.1039/B202464K

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