• Media type: E-Article
  • Title: The formation of dimers and trimers in free jet He4 cryogenic expansions
  • Contributor: Bruch, Ludwig W.; Schöllkopf, Wieland; Toennies, J. Peter
  • imprint: AIP Publishing, 2002
  • Published in: The Journal of Chemical Physics
  • Language: English
  • DOI: 10.1063/1.1486442
  • ISSN: 0021-9606; 1089-7690
  • Keywords: Physical and Theoretical Chemistry ; General Physics and Astronomy
  • Origination:
  • Footnote:
  • Description: <jats:p>The formation of dimers, trimers, and tetramers in a free jet cryogenic expansion of He4 atoms has been studied by diffraction from a nanostructure transmission grating. The final average velocities, speed ratios and ambient temperatures of the expansions for source temperatures of 30, 12, and 6 K and source pressures between 0.1 and 80 bar were determined from time-of-flight measurements of the He atoms. The final mole fractions of the He2, He3, and He4 clusters in the beam were determined from the intensities of the corresponding first-order diffraction peaks for the same range of source conditions. For each source temperature, the final mole fractions of these small clusters first rise, pass through a maximum and then decrease with increasing source pressure. The processes leading to the formation of these clusters are simulated with a kinetic model that allows for density and temperature changes in the expanding beam. The best-fit three-body recombination rate constant for dimer formation increases by over three orders of magnitude as the thermal energy decreases from 1 K to 1 mK, in qualitative agreement with recent theories.</jats:p>