Abstract
High resolution inelastic neutron scattering (INS) measurements of the low temperature (T∼2.0K) rotational dynamics of isotopically substituted methane monolayers adsorbed on MgO(100) are presented. These spectra, obtained using BASIS at SNS, represent the most detailed measurements available for surface-adsorbed monolayer films of methane. Distinct excitations are readily observed at 15, 31, 45 and 127μeV for the CH2D2 on MgO monolayer and at 40, 51, 95 and 138μeV for CH3D/MgO. These features are attributed to tunneling transitions between sublevels within the ground librational state and are interpreted using the pocket state (PS) formalism first proposed by Hüller. This theoretical analysis employs the findings of earlier studies of CH4 on MgO(100) which suggest that molecules adsorb with their C2v axes normal to the surface plane. The comparison between theory and experiment provides direct insight into the impact of molecular versus surface symmetry on the observed tunneling spectra.
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