Time-resolved low energy photoelectron diffraction for the study of surface structural dynamics with sub-100 fs temporal resolution

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Based on the diffraction of low energy photoelectrons we aim for proving and applying a novel experimental concept for the study of ultrafast structural dynamics at surfaces with sub-100 fs temporal resolution. Next to structural information, the detected transient photoemission signal will at the same time carry information about excitation and relaxation of the involved surface electronic system potentially allowing for a direct correlation of structural and carrier dynamics at surfaces. Within our studies we will focus on sub-monolayer adsorption of phthalocyanine molecules on noble metal surfaces. The distinctive low energy photoelectron diffraction patterns that have been reported for different representatives of this adsorbate-surface system in static ARPES experiments represent an ideal test bed for the examination of the capabilities and limitations of the proposed concept. Furthermore, we expect that the combined interrogation of structural and carrier dynamics can shed new light into the complex interaction mechanisms governing the multifaceted properties of this metal-organic interface class. Two different experimental configurations will be realized and tested within the project: In using 70 fs NUV laser pulses (6 eV) for the generation of the probing photoelectrons we will be able to probe structural and carrier dynamics at an ultimate temporal resolution below 100 fs. The intrinsic very low kinetic energies of the photoelectrons of Ekin < 2 eV will, however, limit our studies to small and moderate pump fluences due to a signal background arising from pump-induced parasitic electron emission. In an alternative configuration we will use 18 eV vacuum ultraviolet pulses from a HHG source so that also experiments at significantly higher pump fluences will become possible. In this fluence regime we expect to be able to trigger also structural phase transitions in the adsorbate layer.