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A central motivation for the development of x-ray free-electron lasers has been the prospect of time-resolved single-molecule imaging with atomic resolution. Here, we show that x-ray photoelectron diffraction—where a photoelectron emitted after x-ray absorption illuminates the molecular structure from within—can be used to image the increase of the internuclear distance during the x-ray-induced fragmentation of an O2 molecule. By measuring the molecular-frame photoelectron emission patterns for a two-photon sequential K-shell ionization in coincidence with the fragment ions, and by sorting the data as a function of the measured kinetic energy release, we can resolve the elongation of the molecular bond by approximately 1.2 a.u. within the duration of the x-ray pulse. The experiment paves the road toward time-resolved pump-probe photoelectron diffraction imaging at high-repetition-rate x-ray free-electron lasers.
In this paper, the concepts of microscopic transport theory are introduced and the features and shortcomings of the most commonly used ansatzes are discussed. In particular, the Ultrarelativistic Quantum Molecular Dynamics (UrQMD) transport model is described in great detail. Based on the same principles as QMD and RQMD, it incorporates a vastly extended collision term with full baryon-antibaryon symmetry, 55 baryon and 32 meson species. Isospin is explicitly treated for all hadrons. The range of applicability stretches from E lab < 100$ MeV/nucleon up to E lab> 200$ GeV/nucleon, allowing for a consistent calculation of excitation functions from the intermediate energy domain up to ultrarelativistic energies. The main physics topics under discussion are stopping, particle production and collective flow.