Valence-Electron Resonances in Alkali-Metal Overlayers Observed via Photoemission Line-Shape Changes

Valence-electron resonances for Na overlayers on Ag(111) and Cu(111) are observed by photoemission via line-shape changes for the substrate s,p-band emission in a narrow range of photon energies. The effect is ascribed to interfering contributions to the photoelectron wave from the substrate and the vacuum barrier

Coverage-dependent frequency for Li-atom vibrations on Cu(111)

Electron-energy-loss spectra recorded for monolayer amounts of Li adsorbed on Cu(111) show a loss peak associated with Li vibrations perpendicular to the substrate. The loss energy shifts from 38 meV at low coverage to 43 meV at 0.3 ML and remains constant for coverages between 0.3 and 0.5 ML. The loss intensity passes a maximum at a Li coverage of 0.15 ML and gradually decreases such that it is difficult to resolve a loss peak at coverages above 0.5 ML. The high loss energy indicates that the adatom resides on the surfaces rather than in substitutional sites. The frequency shift is much too large to be explained by dipole-dipole interactions. The above results are obtained with the evaporation source loaded with the natural Li isotope mixture (92.6% 7Li, 7.4% 6Li). Measurements with 6Li show that the increase of the vibration frequency with increasing coverage is not an isotope effect

Observation of structure changes for Li/Cu(111) by photoemission from Li core and quantum-well states

Via photoemission from discrete quantum-well valence states and the Li 1s core level, three different types of atom rearrangements are observed for Cu(111)/Li. In the monolayer coverage range gradual energy shifts for the core-level as well as a quantum-well state reflect a gradual lateral compression of the Li overlayer as more atoms are adsorbed. The onset of Li substitution and formation of a (2×2) structure when, at RT, monolayer Li coverage is exceeded, is monitored via the disappearance and appearance of quantum-well states characteristic of the adsorbed full monolayer of Li and the part substitutional (2×2) structure, respectively. A splitting of the Li 1s emission peak into a doublet reflects the two different Li sites characteristic of the (2×2) phase. A small energy shift of the quantum-well state (25 meV) indicates that, if it is cooled (170 K), the substitutional structure is unstable with respect to Li adsorption

Oscillatory photoemission cross section for simple-metal quantum wells

A strong, oscillatory photon energy dependence is observed for the intensity of photoemission peaks due to quantum-well states in Na overlayers on Cu(111). The measurements are made at low photon energies (hν<8 eV) with Na films, which are between four and eight atomic layers thick. The intensity oscillations are ascribed to the interference between the contributions to the outgoing wave associated with the two tails of a quantum-well state

Shifts and widths of metal-overlayer quantum-well states near EF observed by photoemission

Photoelectron energy spectra reveal discrete valence-electron states in the range 0–220 meV above EF for 1–3 atomic layers of Na on Cu(111). Apart from a stepwise dependence on the number of atomic Na layers the energy of the quantum-well states depends in a gradual manner on how full the layer is. The states are as well defined in energy as comparable surface states producing peak widths (50–90 meV), which depend on temperature and coverage

Overlayer resonance and quantum well state of Cs/Cu(111) studied with angle-resolved photoemission, LEED, and first-principles calculations

Angle-resolved photoemission spectroscopy and low-energy electron diffraction are used to study submonolayer coverages of Cs on Cu(111) at room temperature (RT) and 170 K. At RT, the Cs saturation coverage is approximately 90% of the full monolayer coverage. The full monolayer is characterized by a quantum well state (QWS) band having an energy of 25 meV below the Fermi level (E-F) in the (Gamma) over bar point and a resonance band extending to energies below the Cu band gap. This is supported by our first-principles calculations. Low-energy electron diffraction shows that the Cs overalyer forms a (2x2) structure over a wide coverage range, in which the QWS has energies from 50 meV above to 25 meV below E-F. The continued energy shift of the QWS after saturation of the diffraction angles is interpreted in terms of vacancies in the overlayer

Structure changes for Cu(111)/Li observed via discrete quantum well states

Via photoemission in the near UV from discrete quantum well states, four different types of atom rearrangements are observed for Cu(111)/Li. In the monolayer range a gradual energy shift reflects a gradual compression of the Li layer as more atoms are adsorbed. The onset of Li substitution and formation of a (2×2) structure when, at RT, monolayer Li coverage is exceeded is monitored via the appearance of a quantum well state characteristic of the new phase. A small energy shift indicates that, if it is cooled (170 K), the new structure is unstable with respect to Li adsorption. Finally, an energy downshift with increasing coverage observed for a state characteristic of 2 ML Li is ascribed to an increasing area for one-atomic-layer-high islands formed by Li atoms on top of the first full layer

Oscillatory photoemission cross section for alkali monolayer quantum well states

A strong oscillatory photon energy dependence, observed in the photon energy range between 5 and 26 eV, for the intensity of photoemission peaks due to quantum well states in Na and Cs monolayers on Cu(111) is ascribed to interference between the contributions to the outgoing photoelectron wave from the two tails of the quantum well state