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.

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Journal 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