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We describe the results of experiments and simulations performed with the aimof extending photoelectron spectroscopy with intense laser pulses to the caseof molecular compounds. Dimer frame photoelectron angular distributionsgenerated by double ionization of N$_2$-N$_2$ and N$_2$-O$_2$ van der Waalsdimers with ultrashort, intense laser pulses are measured using four-bodycoincidence imaging with a reaction microscope. To study the influence of thefirst-generated molecular ion on the ionization behavior of the remainingneutral molecule we employ a two-pulse sequence comprising of a linearlypolarized and a delayed elliptically polarized laser pulse that allowsdistinguishing the two ionization steps. By analysis of the obtained electronmomentum distributions we show that scattering of the photoelectron on theneighbouring molecular potential leads to a deformation and rotation of thephotoelectron angular distribution as compared to that measured for an isolatedmolecule. Based on this result we demonstrate that the electron momentum spacein the dimer case can be separated, allowing to extract information about theionization pathway from the photoelectron angular distributions. Our work, whenimplemented with variable pulse delay, opens up the possibility ofinvestigating light-induced electronic dynamics in molecular dimers usingangularly resolved photoelectron spectroscopy with intense laser pulses.

Exploring photoelectron angular distributions emitted from molecular dimers by two delayed intense laser pulses