Molecular Movies from Molecular Frame Photoelectron Angular Distribution (MF-PAD) Measurements

We discuss recent and on-going experiments, where molecular frame photoelectron angular distributions (MFPADs) of high kinetic energy photoelectrons are measured in order to determine the time evolution of molecular structures in the course of a photochemical event. These experiments include, on the one hand, measurements where single XUV/X-ray photons, obtained from a free electron laser (FEL) or by means of high-harmonic generation (HHG), are used to eject a high energy photoelectron, and, on the other hand, measurements where a large number of mid-infrared photons are absorbed in the course of strong-field ionization. In the former case, first results indicate a manifestation of the both the electronic orbital and the molecular structure in the angle-resolved photoelectron distributions, while in the latter case novel holographic structures are measured that suggest that both the molecular structure and ultrafast electronic rearrangement processes can be studied with a time-resolution that reaches down into the attosecond and few-femtosecond domain