Abstract
When an internal mode of an absorbate is excited with enough energy to break the absorbate-surface bond, the adsorbate may desorb in a manner similar to predissociation (or unimolecular reaction) in isolated molecules. In this article, we set up a simple, microscopic model for this " predesorption" process and investigate the influence of various aspects of the model on the time scale of predesorption. These comparisons include quantum mechanical vs classical treatment, and the inclusion vs neglect of surface vibrations. For this simple analog of a "unimolecular reaction," we find that classical mechanics predicts shorter lifetimes; and that the effect of surface vibrations is far less pronounced in quantum mechanics.
| Original language | English |
|---|---|
| Pages (from-to) | 1968-1973 |
| Number of pages | 6 |
| Journal | Journal of Chemical Physics |
| Volume | 90 |
| Issue number | 3 |
| Publication status | Published - 1989 |
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ASJC Scopus subject areas
- Atomic and Molecular Physics, and Optics
Cite this
A theoretical investigation of microscopic dynamics and time scales of predesorption processes. / Muckerman, James; Uzer, T.
In: Journal of Chemical Physics, Vol. 90, No. 3, 1989, p. 1968-1973.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - A theoretical investigation of microscopic dynamics and time scales of predesorption processes
AU - Muckerman, James
AU - Uzer, T.
PY - 1989
Y1 - 1989
N2 - When an internal mode of an absorbate is excited with enough energy to break the absorbate-surface bond, the adsorbate may desorb in a manner similar to predissociation (or unimolecular reaction) in isolated molecules. In this article, we set up a simple, microscopic model for this " predesorption" process and investigate the influence of various aspects of the model on the time scale of predesorption. These comparisons include quantum mechanical vs classical treatment, and the inclusion vs neglect of surface vibrations. For this simple analog of a "unimolecular reaction," we find that classical mechanics predicts shorter lifetimes; and that the effect of surface vibrations is far less pronounced in quantum mechanics.
AB - When an internal mode of an absorbate is excited with enough energy to break the absorbate-surface bond, the adsorbate may desorb in a manner similar to predissociation (or unimolecular reaction) in isolated molecules. In this article, we set up a simple, microscopic model for this " predesorption" process and investigate the influence of various aspects of the model on the time scale of predesorption. These comparisons include quantum mechanical vs classical treatment, and the inclusion vs neglect of surface vibrations. For this simple analog of a "unimolecular reaction," we find that classical mechanics predicts shorter lifetimes; and that the effect of surface vibrations is far less pronounced in quantum mechanics.
UR - http://www.scopus.com/inward/record.url?scp=0000498986&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=0000498986&partnerID=8YFLogxK
M3 - Article
VL - 90
SP - 1968
EP - 1973
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 3
ER -