Table of Contents:
Image-potential resonances on the (100) surface of pure Aluminum are investigated experimentally and theoretically. The experiments are conducted both energy- and time-resolved using the method of two-photon photoemission spectroscopy. The main attention of the theoretical examination and extensive numerical calculations is devoted to the interaction between surface and bulk states. Image-potential resonances on Al(100) are a system in which a complete series of discrete Rydberg states strongly couples to a continuum of states. As a simple metal it also provides a good opportunity to test theoretical models of the structure of the potential at metal surfaces. This work represents the first high-resolution investigation of image-potential resonances with such strong resonance character.
For the first time, it is demonstrated experimentally that isolated image-potential resonances exist on an Aluminum surface. On the (100) surface of Aluminum the second through fifth image-potential resonance are resolved and both, their energies and lifetimes are measured. The binding energies of the image-potential resonances form a Rydberg series of states. Within the accuracy of the measurement it is not necessary to introduce a quantum defect a (a=0.022±0.035). Using angle-resolved two-photon photoemission spectroscopy the effective mass of electrons in the second image-potential resonance is measured to 1.01±0.11 electron masses.
The lifetimes of the resonances increase as (1.0±0.2)·n³ fs starting from n=2. Calculations using the density matrix formalism show that the experimentally observed lifetimes can be explained well by electrons decaying into the bulk. The effect of resonance trapping leads to extended lifetimes in the process.
Contrary to common theoretical models of image-potential states at metal surfaces the first image-potential resonance cannot be observed in two-photon photoemission on Al(100). It is shown that this result can be explained by the strong coupling of the surface states to bulk states which causes the trapping of resonances. The Fano effect can be observed in energy dependent two-photon photoemission spectra. It becomes evident through a strong asymmetry between signal intensities at energies below and above the series of resonances.