Dynamics of Kr in dense clathrate hydrates.
- X-Ray Science Division
The dynamics of Kr atoms as guests in dense clathrate hydrate structures are investigated using site specific {sup 83}Kr nuclear resonant inelastic x-ray scattering (NRIXS) spectroscopy in combination with molecular dynamics simulations. The dense structure H hydrate and filled-ice structures are studied at high pressures in a diamond anvil high-pressure cell. The dynamics of Kr in the structure H clathrate hydrate quench recovered at 77 K is also investigated. The Kr phonon density of states obtained from the experimental NRIXS data are compared with molecular dynamics simulations. The temperature and pressure dependence of the phonon spectra provide details of the Kr dynamics in the clathrate hydrate cages. Comparison with the dynamics of Kr atoms in the low-pressure structure II obtained previously was made. The Lamb-Mossbauer factor obtained from NRIXS experiments and molecular dynamics calculations are in excellent agreement and are shown to yield unique information on the strength and temperature dependence of guest-host interactions.
- Research Organization:
- Argonne National Laboratory (ANL)
- Sponsoring Organization:
- SC
- DOE Contract Number:
- AC02-06CH11357
- OSTI ID:
- 1015965
- Report Number(s):
- ANL/XSD/JA-70238
- Journal Information:
- Phys. Rev. B, Journal Name: Phys. Rev. B Journal Issue: 2011 Vol. 83; ISSN 1098-0121
- Country of Publication:
- United States
- Language:
- ENGLISH
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