We report inelastic neutron scattering experiments from natural methane hyd
rates sampled from the Pacific sea-floor during an expedition of the resear
ch ship SONNE. The experiments verify directly the content of methane by me
asuring the rotational spectrum of the CH4 molecules. The existence of almo
st free rotational levels excludes off-center positions of the molecules in
the cages. In addition we could assign the observed peaks in the energy re
gime up to 5 meV to rotational excitations only. The observed relative shar
p excitations prove a surprisingly good crystallinity of the geological sam
ple. The finite width is attributed to frozen-in hydrogen disorder of the i
ce cages.