Coherence in Molecular Photoionization

Abstract: The development of attosecond technology has enabled the real-time observation of coherent electron motion in atoms, molecules and condensed phases. Experimentally, it is now possible to generate laser pulses of durations of only a few tens of attoseconds. These durations are of the order of the revolution period of the first Bohr orbit (150 asec), opening the way to visualize and even control electron dynamics at its natural time scale. This PhD thesis constitutes a theoretical study of fundamental phenomena occurring in gas-phase molecules upon interaction with light. We have investigated ultrafast charge migration in biological molecules initiated by attosecond XUV pulses. In addition, we have studied the high-energy interferences that arise in the vibrationally-resolved photoelectron spectra of small polyatomic molecules. In order to explore these complex phenomena, we have employed numerical methods that describe molecular photoionization by evaluating continuum scattering wave functions, allowing us to compute different observables such as time-dependent electron densities or photoionization cross sections.