Recent progress in laser science allows the creation of femto- to attosecond X-ray light pulses and paves the way for a completely new generation of experiments investigating ultrafast processes in biology, chemistry and physics. Intensive research efforts worldwide are pursuing the implementation of “pilot” experiments that demonstrate the scientific potential of this area. However, the challenging nature of femtosecond X-ray sources requires experts with interdisciplinary training in X-ray laser-science and in the research areas that can benefit from its use. The goal of the proposed project is to develop and establish X-ray pump-probe spectroscopies using high-harmonic light sources to study femtosecond surface dynamics. Three ultrafast surface science areas will be addressed: surface magnetism, chemical reactions and phase transitions. The proposed interdisciplinary experiments will yield new insight in femtosecond quasiparticle interactions and will also impact possible applications in magnetic memory production, catalysis and organic materials. The applicant is an expert in surface science, who will complement his skills in organic materials, femtochemistry and high-harmonic X-ray generation with the Kapteyn-Murnane Group at JILA (USA), who are leading scientists in the field. The proposed project is at the cutting edge of ultrafast surface science and will promote EU research in this field during the return phase with Prof. Aeschlimann (GER) at the University of Kaiserslautern, who is one of the global key opinion leaders for ultrafast phenomena. The proposed project will help the fellow researcher gain professional maturity and to actively participate in shaping the next generation of ultrafast research with X-ray pulses, an area that is rapidly expanding with increasing worldwide availability of high harmonic and free electron laser light sources.