AbstractWe present the results of an investigation into the interaction of SF_6 molecules and clusters in a molecular beam with resonant IR laser radiation at different stages of the beam evolution along the axis of its propagation. The beam has been formed as a result of gas-dynamic expansion of a mixture of SF_6 with argon carrier gas during expansion from a pulsed nozzle. The experimental setup and the investigation method are described. It has been shown that selective vibrational excitation of SF_6 molecules with a specific sulfur isotope by a CO_2 laser near the nozzle edge causes suppression of the clustering process of these isotopic molecules. Selective IR excitation of clusters under the conditions of the formed cluster beam leads to isotopically selective dissociation of clusters. Depending on the experimental conditions including different distances of the irradiation zone of particles from the nozzle edge, the results of measuring the efficiency and selectivity of molecular clustering suppression and cluster dissociation processes are presented. It has been shown that both of these processes make it possible to achieve high selectivity values for the ^32S and ^34S sulfur isotopes. In the case in which the clustering of SF_6 molecules was selectively suppressed, selectivity values α ≥ 25–30 have been obtained. Upon selective dissociation of (SF_6)_2 dimers under similar expansion conditions of the gas mixture, selectivity values α ≥ 20–25 for ^32SF_6^32SF_6 dimers with respect to ^34SF_6^32SF_6 dimers have been obtained. Particular attention has been paid to measurements at a high dilution of SF_6 in argon under conditions of predominant formation of (SF_6)_ m Ar_ n mixed clusters. The potential of using studied processes as a basis for the technology of the laser isotope separation are discussed.

The composition and content of pulsed neutral cluster beams are determined by a specially proposed method from ion signals of cluster fragments in time-of-flight spectra of clusters in these beams. For beams of different-size mixed clusters (SF 6 ) m Ar n (where 1 ≤ m ≤ 4 and 0 ≤ n ≤ 9 are the number of molecules and atoms in clusters, respectively), it is shown that the proposed method makes it possible to determine the composition and content of neutral van der Waals molecular and atomic–molecular clusters in beams.