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| Content Provider | PubMed Central |
|---|---|
| Author | Crim, F. Fleming |
| Abstract | Experimental studies of the chemical reaction dynamics of vibrationally excited molecules reveal the ability of different vibrations to control the course of a reaction. This Perspective describes those studies for the prototypical reaction of vibrationally excited methane and its isotopologues in gases and on surfaces and looks to the prospects of similar studies in liquids. The influences of vibrational excitation on the CH bond cleavage in a single collision reaction with Cl and in dissociative adsorption on a Ni surface bear some striking similarities. Both reactions are bond-selective processes in which the initial preparation of a molecular eigenstate containing a large component of CH stretching results in preferential cleavage of that bond. It is possible to cleave either the CH bond or CD bond in the reaction of Cl with CH3D, CH2D2, or CHD3 and, similarly, to use initial excitation of the CH stretch to promote dissociation of CHD3 to CD3 and H on a Ni surface. Different vibrational modes, such as the symmetric and antisymmetric stretches in CH3D or CH4, lead to very different reactivities, and molecules with the symmetric stretching vibration excited can be as much as 10 times more reactive than ones with the antisymmetric stretch excited. The origin of this behavior lies in the change in the vibrational motion induced by the interaction with the atomic reaction partner or the surface. |
| Related Links | http://dx.doi.org/10.1073/pnas.0803010105 |
| Ending Page | 12661 |
| Page Count | 8 |
| Starting Page | 12654 |
| File Format | |
| ISSN | 00278424 |
| e-ISSN | 10916490 |
| Journal | Proceedings of the National Academy of Sciences of the United States of America |
| Issue Number | 35 |
| Volume Number | 105 |
| Language | English |
| Publisher | National Academy of Sciences |
| Publisher Date | 2008-09-02 |
| Access Restriction | Open |
| Rights Holder | National Academy of Sciences |
| Subject Keyword | General Research in Higher Education |
| Content Type | Text |
| Resource Type | Article |
| Subject | Multidisciplinary |
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