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The one-phonon inelastic low energy helium atom scattering theory is adapted to cases where the target monolayer is a p(1x1) commensurate square lattice. Experimental data for para-H2/NaCl(001) are re-analyzed and the relative intensities of energy loss peaks in the range 6 to 9 meV are determined. The case of the H2/NaCl(001) monolayer for 26 meV scattering energy is computationally challenging and difficult because it has a much more corrugated surface than those in the previous applications for triangular lattices. This requires a large number of coupled channels for convergence in the wave-packet-scattering calculation and a long series of Fourier amplitudes to represent the helium-target potential energy surface. A modified series is constructed in which a truncated Fourier expansion of the potential is constrained to give the exact value of the potential at some key points and which mimics the potential with fewer Fourier amplitudes. The shear horizontal phonon mode is again accessed by the helium scattering for small misalignment of the scattering plane relative to symmetry axes of the monolayer. For 1° misalignment, the calculated intensity of the longitudinal acoustic phonon mode frequently is higher than that of the shear horizontal phonon mode in contrast to what was found at scattering energies near 10 meV for triangular lattices of Ar, Kr, and Xe on Pt(111).

The adsorption of water on r-TiO2(110) has been investigated with thermal desorption spectroscopy (TDS) and helium atom scattering. Conventional TDS using a mass spectrometer and He-TDS monitoring reflected He beam intensity consistently show the existence of a structurally well-defined monolayer as well as a highly ordered second layer of water and a disordered multilayer phase. He diffraction patterns recorded along the high symmetry [001], equation image, and equation image directions reveal a well-ordered superstructure with (1x1) symmetry, providing strong evidence for the absence of a partially dissociated monolayer on the perfect parts of the substrate. No changes in the diffraction patterns are observed after irradiation with UV-light.

Under ambient conditions, almost all metals are coated by an oxide. These coatings, the result of a chemical reaction, are not passive. Many of them bind, activate and modify adsorbed molecules, processes that are exploited, for example, in heterogeneous catalysis and photochemistry. Here we report an effect of general importance that governs the bonding, structure formation and dissociation of molecules on oxidic substrates. For a specific example, methanol adsorbed on the rutile TiO2(110) single crystal surface, we demonstrate by using a combination of experimental and theoretical techniques that strongly bonding adsorbates can lift surface relaxations beyond their adsorption site, which leads to a sig- nificant substrate-mediated interaction between adsorbates. The result is a complex super- structure consisting of pairs of methanol molecules and unoccupied adsorption sites. Infrared spectroscopy reveals that the paired methanol molecules remain intact and do not depro- tonate on the defect-free terraces of the rutile TiO2(110) surface.