Bonn, Mischa ; Hess, Christian ; Wolf, Martin (2024)
The dynamics of vibrational excitations on surfaces: CO on Ru(001).
In: The Journal of Chemical Physics, 2001, 115 (16)
doi: 10.26083/tuprints-00026897
Artikel, Zweitveröffentlichung, Verlagsversion
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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: | 2024 |
| Autor(en): | Bonn, Mischa ; Hess, Christian ; Wolf, Martin |
| Art des Eintrags: | Zweitveröffentlichung |
| Titel: | The dynamics of vibrational excitations on surfaces: CO on Ru(001) |
| Sprache: | Englisch |
| Publikationsjahr: | 23 April 2024 |
| Ort: | Darmstadt |
| Publikationsdatum der Erstveröffentlichung: | 2001 |
| Ort der Erstveröffentlichung: | 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: | 10.26083/tuprints-00026897 |
| URL / URN: | https://tuprints.ulb.tu-darmstadt.de/26897 |
| Zugehörige Links: | |
| Herkunft: | Zweitveröffentlichungsservice |
| 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. |
| Status: | Verlagsversion |
| URN: | urn:nbn:de:tuda-tuprints-268972 |
| Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 500 Naturwissenschaften und Mathematik > 530 Physik 500 Naturwissenschaften und Mathematik > 540 Chemie |
| Hinterlegungsdatum: | 23 Apr 2024 08:32 |
| Letzte Änderung: | 24 Apr 2024 14:30 |
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| Suche nach Titel in: | TUfind oder in Google |
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