Cho, Minhaeng ; Hess, Christian ; Bonn, Mischa (2002)
Lateral interactions between adsorbed molecules: Investigations of CO on Ru(001) using nonlinear surface vibrational spectroscopies.
In: Physical Review B, 65 (20)
doi: 10.1103/PhysRevB.65.205423
Artikel, Bibliographie
Dies ist die neueste Version dieses Eintrags.
Kurzbeschreibung (Abstract)
We present an experimental and theoretical investigation into the coupling of C-O stretch vibrations of CO molecules adsorbed on Ru(001). We employ surface infrared-visible (IR-VIS) (IV) and infrared-infrared-visible (IR-IR-VIS) (IIV) sum-frequency generation (SFG) (IV-SFG and IIV-SFG, respectively) to investigate the effects of the intermolecular coupling through the nonlinear optical response of the system. As a consequence of the increased intermolecular interaction with increasing coverage due to the closer proximity of CO molecules on the surface, we observe pronounced frequency shifts of the vibrational resonances. In addition, the intensity behavior in both the IV-SFG and IIV-SFG spectra exhibits a strong nonlinear dependence on the coverage. These observations can be reproduced by extending previous theories for the coverage-dependent linear optical response (used to explain IR reflectance absorption data) to the nonlinear optical response. Expressions are derived for the second- and third-order nonlinear susceptibilities in terms of molecular properties such as the polarizability, hyperpolarizability, and second hyperpolarizability. We obtain very good quantitative agreement between theory and experiment. The analysis indicates that the principal effect of the intermolecular coupling on the nonlinear optical response is through a local-field correction for the linear IR field.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2002 |
| Autor(en): | Cho, Minhaeng ; Hess, Christian ; Bonn, Mischa |
| Art des Eintrags: | Bibliographie |
| Titel: | Lateral interactions between adsorbed molecules: Investigations of CO on Ru(001) using nonlinear surface vibrational spectroscopies |
| Sprache: | Englisch |
| Publikationsjahr: | 2002 |
| Ort: | College Park, MD |
| Verlag: | American Physical Society |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Physical Review B |
| Jahrgang/Volume einer Zeitschrift: | 65 |
| (Heft-)Nummer: | 20 |
| Kollation: | 10 Seiten |
| DOI: | 10.1103/PhysRevB.65.205423 |
| Zugehörige Links: | |
| Kurzbeschreibung (Abstract): | We present an experimental and theoretical investigation into the coupling of C-O stretch vibrations of CO molecules adsorbed on Ru(001). We employ surface infrared-visible (IR-VIS) (IV) and infrared-infrared-visible (IR-IR-VIS) (IIV) sum-frequency generation (SFG) (IV-SFG and IIV-SFG, respectively) to investigate the effects of the intermolecular coupling through the nonlinear optical response of the system. As a consequence of the increased intermolecular interaction with increasing coverage due to the closer proximity of CO molecules on the surface, we observe pronounced frequency shifts of the vibrational resonances. In addition, the intensity behavior in both the IV-SFG and IIV-SFG spectra exhibits a strong nonlinear dependence on the coverage. These observations can be reproduced by extending previous theories for the coverage-dependent linear optical response (used to explain IR reflectance absorption data) to the nonlinear optical response. Expressions are derived for the second- and third-order nonlinear susceptibilities in terms of molecular properties such as the polarizability, hyperpolarizability, and second hyperpolarizability. We obtain very good quantitative agreement between theory and experiment. The analysis indicates that the principal effect of the intermolecular coupling on the nonlinear optical response is through a local-field correction for the linear IR field. |
| ID-Nummer: | Artikel-ID: 205423 |
| Hinterlegungsdatum: | 29 Okt 2010 10:00 |
| Letzte Änderung: | 24 Apr 2024 14:35 |
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| Suche nach Titel in: | TUfind oder in Google |
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Lateral interactions between adsorbed molecules: Investigations of CO on Ru(001) using nonlinear surface vibrational spectroscopies. (deposited 23 Apr 2024 08:38)
- Lateral interactions between adsorbed molecules: Investigations of CO on Ru(001) using nonlinear surface vibrational spectroscopies. (deposited 29 Okt 2010 10:00) [Gegenwärtig angezeigt]
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