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- W2071003325 abstract "Raman spectroscopic measurements of simple hydrogen and tetrahydrofuran+hydrogen sII clathrate hydrates have been performed. Both the roton and vibron bands illuminate interesting quantum dynamics of enclathrated H2 molecules. The complex vibron region of the Raman spectrum has been interpreted by observing the change in population of these bands with temperature, measuring the absolute H2 content as a function of pressure, and with D2 isotopic substitution. Quadruple occupancy of the large sII clathrate cavity shows the highest H2 vibrational frequency, followed by triple and double occupancies. Singly occupied small cavities display the lowest vibrational frequency. The vibrational frequencies of H2 within all cavity environments are redshifted from the free gas phase value. At 76 K, the progression from ortho- to para-H2 occurs over a relatively slow time period (days). The rotational degeneracy of H2 molecules within the clathrate cavities is lifted, observed directly in splitting of the para-H2 roton band. Raman spectra from H2 and D2 hydrates suggest that the occupancy patterns between the two hydrates are analogous, increasing confidence that D2 is a suitable substitute for H2. The measurements suggest that Raman is an effective and convenient method to determine the relative occupancy of hydrogen molecules in different clathrate cavities." @default.
- W2071003325 created "2016-06-24" @default.
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- W2071003325 date "2009-01-06" @default.
- W2071003325 modified "2023-09-27" @default.
- W2071003325 title "Raman spectroscopic studies of hydrogen clathrate hydrates" @default.
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- W2071003325 doi "https://doi.org/10.1063/1.3046678" @default.
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