  We theoretically study how time- and angle-resolved photoemission
spectroscopy can be applied for imaging coherent electron dynamics in
molecules. We consider a process in which a pump pulse triggers coherent
electronic dynamics in a molecule by creating a valence electron hole. An
ultrashort extreme ultraviolet (XUV) probe pulse creates a second electron hole
in the molecule. Information about the electron dynamics is accessed by
analyzing angular distributions of photoemission probabilities at a fixed
photoelectron energy. We demonstrate that a rigorous theoretical analysis,
which takes into account the indistinguishability of transitions induced by the
ultrashort, broadband probe pulse and electron hole correlation effects, is
necessary for the interpretation of time- and angle-resolved photoelectron
spectra. We show how a Fourier analysis of time- and angle-resolved
photoelectron spectra from a molecule can be applied to follow its electron
dynamics by considering photoelectron distributions from an indole molecular
cation with coherent electron dynamics.
