Detailed study of pure methane hydrate in a diamond cell with in situ optic
al, Raman, and x-ray microprobe techniques reveals two previously unknown s
tructures, structure II and structure H, at high pressures. The structure I
l methane hydrate at 250 MPa has a cubic unit cell of a = 17.158(2) Angstro
m and volume V = 5051.3(13) Angstrom (3); structure H at 600 MPa has a hexa
gonal unit cell of a = 11.980(2) A, c = 9.992(3) Angstrom, and V = 1241.9(5
) Angstrom (3). The compositions of these two investigated phases are still
not known. With the effects of pressure and the presence of other gases in
the structure, the structure Ii phase is likely to dominate over the known
structure I methane hydrate within deep hydrate-bearing sediments underlyi
ng continental margins.