Bonn, Mischa ; Hess, Christian ; Wolf, Martin (2001)
The dynamics of vibrational excitations on surfaces: CO on Ru(001).
In: The Journal of Chemical Physics, 115 (16)
doi: 10.1063/1.1404986
Artikel, Bibliographie
Dies ist die neueste Version dieses Eintrags.
Kurzbeschreibung (Abstract)
We present an experimental and theoretical study of vibrational excitation of the C–O stretch vibration of carbon monoxide adsorbed on a ruthenium Ru(001) surface with ultrashort femtosecond infrared laser pulses. After broadband excitation leading to transfer of a significant fraction of the CO molecules to their first (∼15%) and second (∼5%) vibrationally excited states, we observe a competition between vibrational energy relaxation and energy delocalization through dipole–dipole coupling. We reproduce the observed excited state spectra by solving the three-level Bloch equations and accounting for intermolecular vibrational energy transfer on a picosecond time scale. The rate of vibrational energy transfer, and its coverage-dependence, can be described by a Förster energy transfer mechanism. We discuss possibilities to optimize the degree of localized vibrational excitation of a specific bond of molecules at surfaces through chirped pulse IR excitation.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2001 |
| Autor(en): | Bonn, Mischa ; Hess, Christian ; Wolf, Martin |
| Art des Eintrags: | Bibliographie |
| Titel: | The dynamics of vibrational excitations on surfaces: CO on Ru(001) |
| Sprache: | Englisch |
| Publikationsjahr: | 2001 |
| Ort: | Melville, NY |
| Verlag: | AIP Publishing |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | The Journal of Chemical Physics |
| Jahrgang/Volume einer Zeitschrift: | 115 |
| (Heft-)Nummer: | 16 |
| DOI: | 10.1063/1.1404986 |
| Zugehörige Links: | |
| Kurzbeschreibung (Abstract): | We present an experimental and theoretical study of vibrational excitation of the C–O stretch vibration of carbon monoxide adsorbed on a ruthenium Ru(001) surface with ultrashort femtosecond infrared laser pulses. After broadband excitation leading to transfer of a significant fraction of the CO molecules to their first (∼15%) and second (∼5%) vibrationally excited states, we observe a competition between vibrational energy relaxation and energy delocalization through dipole–dipole coupling. We reproduce the observed excited state spectra by solving the three-level Bloch equations and accounting for intermolecular vibrational energy transfer on a picosecond time scale. The rate of vibrational energy transfer, and its coverage-dependence, can be described by a Förster energy transfer mechanism. We discuss possibilities to optimize the degree of localized vibrational excitation of a specific bond of molecules at surfaces through chirped pulse IR excitation. |
| Hinterlegungsdatum: | 04 Nov 2010 15:26 |
| Letzte Änderung: | 24 Apr 2024 14:36 |
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The dynamics of vibrational excitations on surfaces: CO on Ru(001). (deposited 23 Apr 2024 08:32)
- The dynamics of vibrational excitations on surfaces: CO on Ru(001). (deposited 04 Nov 2010 15:26) [Gegenwärtig angezeigt]
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