New extreme-ultraviolet (XUV) light sources such as high-order-harmonic generation (HHG) and free-electron lasers (FELs), combined with laser-induced alignment techniques, enable novel methods for making molecular movies based on measuring molecular frame photoelectron angular distributions. Experiments are presented where CO2 molecules were impulsively aligned using a near-infrared laser and ionized using femtosecond XUV pulses obtained by HHG. Measured electron angular distributions reveal contributions from four orbitals and the onset of the influence of the molecular structure.
Phys. Rev. A

Kelkensberg, F., Rouzée, A., Siu, W., Gademann, G., Johnsson, P., Lucchini, M., … Vrakking, M. J. J. (2011). XUV ionization of aligned molecules. Phys. Rev. A, 84(5, Article number: 51404), 1–4. doi:10.1103/PhysRevA.84.051404