Journal
PHYSICAL REVIEW LETTERS
Volume 93, Issue 12, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.93.125503
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The D-2 clathrate hydrate crystal structure was determined as a function of temperature and pressure by neutron diffraction for the first time. The hydrogen occupancy in the (32+X)H-2.136H(2)O, x=0-16 clathrate can be reversibly varied by changing the large (hexakaidecahedral) cage occupancy between two and four molecules, while remaining single occupancy of the small (dodecahedral) cage. Above 130-160 K, the guest D-2 molecules were found in the delocalized state, rotating around the centers of the cages. Decrease of temperature results in rotation freezing followed by a complete localization below 50 K.
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