New insight into ever smaller microscopic units of matter as well as in ever faster evolving chemical, physical or atomic processes pushes the frontiers in many fields in science. Pump/probe experiments turned out to be the most direct approach to time-domain investigations of fast-evolving microscopic processes. Accessing atomic and molecular inner-shell processes directly in the time-domain requires a combination of short wavelengths in the few hundred eV range and sub-femtosecond pulse duration. The concept of light-field-controlled XUV photoemission employs an XUV pulse achieved by High-order Harmonic Generation (HHG) as a pump and the light pulse as a probe or vice versa. The basic prerequisite, namely the generation and measurement of isolated sub-femtosecond XUV pulses synchronized to a strong few-cycle light pulse with attosecond precision, opens up a route to time-resolved inner-shell atomic and molecular spectroscopy with present day sources. Studies of attosecond electronic motion (1 as = 10-18 s) in solids and on surfaces and interfaces have until now remained out of reach. The unprecedented time resolution of the aforementioned technique will enable for the first time monitoring of sub-fs dynamics of such systems in the time domain. These dynamics – of electronic excitation, relaxation, and wave packet motion – are of broad scientific interest and pertinent to the development of many modern technologies including semiconductor and molecular electronics, optoelectronics, information processing, photovoltaics, and optical nano-structuring. The purpose of this project is to investigate phenomena like the temporal evolution of direct photoemission, interference effects in resonant photoemission, fast adsorbate-substrate charge transfer, and electronic dynamics in supramolecular assemblies, in a series of experiments in order to overcome the temporal limits of measurements in solid state physics and to better understand processes in microcosm.
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