Vibrational predissociation of UF6 clusters in supersonic Laval nozzle flow

The time-dependent change in the concentration of UF₆ monomers populated in the ground state was monitored in a supersonic Laval nozzle flow with an infrared diode-laser spectrometer in which the frequency of the laser beam was fixed at the = 1 0 transition (627.7 cm^–1) of the₃ vibrational mode of the²³⁸UF₆ monomer. The concentration of UF₆ monomers in the ground state increased immediately after a single shot from a Raman laser tuned to a vibrational mode of UF₆ clusters (614.8 cm^–1) was applied to the gas in the nozzle. Subsequently, this concentration leveled off and slowly returned to the previous level. These results indicate that the population of UF₆ monomers in the ground state increased as a result of the predissociation of UF₆ clusters vibrationally excited with Raman laser radiation. It is demonstrated that one can utilize this procedure for vibrational predissociation of UF₆ clusters as a technique to increase the concentration of UF₆ monomers in an irradiation zone for molecular laser isotope separation of uranium.