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We have conducted a Raman study of methane (CH4), a major constituent of the outer planets, at pressures up to 165 GPa. We observe splitting of the principal Raman-active vibrational mode above 45 GPa and a nonlinear dependence of Raman peak position on pressure. A discontinuous change in the pressure derivative of the ν3 peak position is observed at approximately 75 GPa, corresponding to the phase change previously observed using X-ray diffraction. The Grüneisen parameters for the principal Raman-active modes of methane in the simple cubic and high-pressure cubic phases are calculated. The predicted dissociation of methane at ultrahigh pressure to form C2H6 and H2 is not observed, but an additional discontinuous change in the pressure-induced shift of the Raman peaks is observed at 110 GPa. We suggest that this may be due to some reorientation or reordering of the methane molecules within the framework of the known cubic lattice. [ABSTRACT FROM AUTHOR]

Ammonia dihydrate (ADH) is an important constituent of the outer solar system and its high-pressure behaviour is relevant to the modelling of Titan, Uranus and Neptune. Our neutron diffraction studies show that ADH can exist at room temperature in the substitutionally disordered structure of the ammonia monohydrate (AMH) phase VI. This implies that a solid solution may exist between ADH and AMH at high pressure, and this is of probable importance to models of the outer solar system. [ABSTRACT FROM AUTHOR]