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Scattering of NH{sub 3} and ND{sub 3} with rare gas atoms at low collision energy

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4935259· OSTI ID:22493219
 [1]
  1. Theoretical Chemistry, Institute for Molecules and Materials, Radboud University, Heyendaalseweg 135, 6525 AJ Nijmegen (Netherlands)

We present a theoretical study of elastic and rotationally inelastic collisions of NH{sub 3} and ND{sub 3} with rare gas atoms (He, Ne, Ar, Kr, Xe) at low energy. Quantum close-coupling calculations have been performed for energies between 0.001 and 300 cm{sup −1}. We focus on collisions in which NH{sub 3} is initially in the upper state of the inversion doublet with j = 1, k = 1, which is the most relevant in an experimental context as it can be trapped electrostatically and Stark-decelerated. We discuss the presence of resonances in the elastic and inelastic cross sections, as well as the trends in the inelastic cross sections along the rare gas series and the differences between NH{sub 3} and ND{sub 3} as a colliding partner. We also demonstrate the importance of explicitly taking into account the umbrella (inversion) motion of NH{sub 3} in order to obtain accurate scattering cross sections at low collision energy. Finally, we investigate the possibility of sympathetic cooling of ammonia using cold or ultracold rare gas atoms. We show that some systems exhibit a large ratio of elastic to inelastic cross sections in the cold regime, which is promising for sympathetic cooling experiments. The close-coupling calculations are based on previously reported ab initio potential energy surfaces for NH{sub 3}–He and NH{sub 3}–Ar, as well as on new, four-dimensional, potential energy surfaces for the interaction of ammonia with Ne, Kr, and Xe, which were computed using the coupled-cluster method and large basis sets. We compare the properties of the potential energy surfaces corresponding to the interaction of ammonia with the various rare gas atoms.

OSTI ID:
22493219
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 18 Vol. 143; ISSN JCPSA6; ISSN 0021-9606
Country of Publication:
United States
Language:
English

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