Ultrafast electron dynamics in Fe(CO)5 and Cr(CO)6 In this thesis the two prototype catalysts Fe(CO)₅ and Cr(CO)₆ are investigated with time resolved photoelectron spectroscopy at a high harmonic setup. In both of these metal carbonyls a UV photon can induce the dissociation of one or more ligands of the complex. The mechanism of the dissociation has been debated over the last decades. The electronic dynamics of the first dissociation occur on the femtosecond timescale. For the experiment an existing high harmonic setup was moved to a new location was extended and characterized. The modified setup can induce dynamics in gas phase samples with photon energies of 1.55eV 3.10eV and 4.65eV. The valence electronic structure of the samples can be probed with photon energies between 20eV and 40eV. The temporal resolution is 111fs to 262fs depending on the combination of the two photon energies. The electronically excited intermediates of the two complexes as well as of the reaction product Fe(CO)₄ could be observed with photoelectron spectroscopy in the gas phase for the first time. ...