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This Historical Account derived in part from D. R. Herschbach was presented as an opening lecture of the Molecular Beam Session organized at the 24th International Symposium on Rarefied Gas Dynamics held in Bari, Italy, in July 2004. The emphasis is on the impressive results due to the molecular beam techniques in the last century. The first section summarizes the historical beam experiments performed by 14 Nobel Prize laureates having used the thermally effusive sources to establish the basic principles of Modern Physics. The second section is on the branching of Molecular Beams to Rarefied Gas Dynamics having permitted to investigate the physics of supersonic free jets and transform the molecular beam techniques. Finally, the last section relates the spectacular molecular beam experiments in helium free jet ultracooling, molecular spectroscopy, chemical reaction dynamics, clustering and modification of low density matter, and biomolecule mass spectrometry, rewarded by nine Nobel Prizes in Chemistry from 1986 to 2002.

The shock wave system of the underexpanded free jet, in a region where the pressure is in the range of 10−2 up to 1 torr, is partly invaded by background molecules, these latter being pumped and carried by the supersonic flow. When a gas mixture is introduced into the nozzle chamber and outside the shock barrel, this aspiration acts very selectively on the light molecules, and a mixture enriched in lighter species is attainable by skimming the free jet. This new aerodynamic separation effect, which is applicable to isotopic mixtures, is very strong in comparison to the efficiency of an elementary gaseous diffusion membrane.