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We use time-resolved momentum microscopy at a free-electron laser (FEL) andextend orbital tomography into the time domain to image the electronic wavefunctions of excited molecular orbitals. This technique provides unprecedentedinsight into the ultrafast interplay between structural and electronicdynamics. In this work we prove general applicability and establish theexperimental conditions at FEL sources to minimize space charge effects andradiation damage. We investigate a bilayer pentacene film on Ag(110) by opticallaser pump and FEL probe experiments. From the momentum microscopy signal, weobtain time-dependent momentum maps of the excited-state dynamics of bothpentacene layers separately. Combining experimental observations with atheoretical study, we interpret the observed signal for the bottom layer asresulting from the charge redistribution between the molecule and the substrateinduced by excitation. We identify that the dynamics of the top pentacene layerresembles excited-state molecular dynamics.

Ultrafast molecular orbital tomography of a pentacene thin film using time-resolved momentum microscopy at a free-electron laser