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Electron localization and solvation in two dimensions

Two–photon photoemission of thiolate/Ag(111), nitrile/Ag(111), and alcohol/Ag(111) interfaces elucidates electron solvation and localization in two dimensions. For low coverages of thiolates on Ag(111), the occupied (HOMO) and unoccupied (LUMO) electronic states of the sulfer–silver bond are localized due to the lattice gas structure of the adsorbate. As the coverage saturates and the adsorbate–adsorbate nearest neighbor distance decreases, the HOMO and LUMO delocalize across many adsorbate molecules. Alcohol– and nitrile–covered Ag(111) surfaces solvate excess image potential state (IPS) electrons. In the case of alcohol–covered surfaces, this solvation is due to a shift in the local workfunction of the surface. For two–monolayer coverages of nitriles/Ag(111), localization accompanies solvation of the IPS. The size of the localized electron can be estimated by Fourier transformation of the wavefunction from momentum– to position–space. The IPS electron localizes to 15±4 Å full-width at half maximum in the plane of the surface, i.e., to a single lattice site.