Ultrafast Dissociation Dynamics Induced in [Fe(CO)5]nXem Mixed Clusters by Resonant Femtosecond Infrared Laser Radiation

ACS Omega. 2022. Vol. 7. No. 50. P. 46203–46212.

Denis G. Poydashev, Ablyasova O., Ryabov E.

Real-time dissociation dynamics induced in [Fe(CO)5]nXem mixed molecular clusters by femtosecond IR radiation in the 5 μm region was studied forthe first time by means of time-resolved methods based on resonant excitation of C
O vibrations in the molecular core of the cluster and photoionization probing (λ = 400 nm) of its decay products. It was found that IR-excited clusters in the initially cold particle beam are heated and dissociated as a result of relaxation processes, giving rise to free neutral Xe aggregates and Fe(CO)5 molecules. Thus, the formed particles are the origin of signal variations from Xe+ and Fe(CO)5+ ions, which grow on a picosecond time scale. It is concluded that the initial laser excitation of C
O vibrations in clusterized molecules is followed by the process of cluster dissociation accompanied with the formation of free neutral particles according to the hierarchy of binding energies: weakly bound shells of Xe atoms are evaporated first and much faster than the Fe(CO)5 molecules from the cluster core. The characteristic times of relaxation processes as well as the cluster temperature were estimated.

Keywords: nanoclusters, intramolecular vibrational redistribution, Femtosecond spectroscopy, intra-cluster dynamics