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We demonstrate the experimental realization of impulsive alignment ofcarbonyl sulfide (OCS) molecules at the Low Density Matter Beamline (LDM) atthe free-electron laser FERMI. OCS molecules in a molecular beam wereimpulsively aligned using 200 fs pulses from a near-infrared laser. Thealignment was probed through time-delayed ionization above the sulphur 2p edge,resulting in multiple ionization via Auger decay and subsequent Coulombexplosion of the molecules. The ionic fragments were collected using atime-of-flight mass spectrometer and the analysis of ion-ion covariance mapsconfirmed the correlation between fragments after Coulomb explosion. Theanalysis of the CO+ and S+ channels allowed us to extract the rotationaldynamics, which is in agreement with our theoretical description as well aswith previous experiments. This result opens the way for a new class ofexperiments at LDM within the field of coherent control of molecules with thepossibilities that a precisely synchronized optical-pump XUV-probe laser setuplike FERMI can offer.

Impulsive laser-induced alignment of OCS molecules at FERMI