A critical comparison of time dependent models for gas–surface sticking

Jackson, Bret
June 1993
Journal of Chemical Physics;6/15/1993, Vol. 98 Issue 12, p9905
Academic Journal
A number of theories describing gas–surface energy transfer are examined. In these theories the gas particle can interact and exchange energy with the vibrational modes of the solid, which are treated quantum mechanically. All of the theories are applied to the same set of model systems, and the results are compared. Probabilities for energy transfer and sticking are computed for He, Ne, and Ar incident on a Cu surface, for a wide range of particle energies and surface temperatures. A recently developed close-coupling approach which includes only single-phonon processes is presented. It is accurate for light particles at low energies and temperatures. Two common approaches to the problem based on an uncorrelated particle–bath state, the forced oscillator and time dependent Hartree methods, are discussed. They are compared with each other and with the close-coupling calculation in the one-phonon limit. Mean field approaches which attempt to improve upon these zero-correlation models are presented and compared with the above models. A new one-phonon multiconfiguration self-consistent field model is also examined.


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