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
Article, Bibliographie
This is the latest version of this item.
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.
| Item Type: | Article |
|---|---|
| Erschienen: | 2002 |
| Creators: | Cho, Minhaeng ; Hess, Christian ; Bonn, Mischa |
| Type of entry: | Bibliographie |
| Title: | Lateral interactions between adsorbed molecules: Investigations of CO on Ru(001) using nonlinear surface vibrational spectroscopies |
| Language: | English |
| Date: | 2002 |
| Place of Publication: | College Park, MD |
| Publisher: | American Physical Society |
| Journal or Publication Title: | Physical Review B |
| Volume of the journal: | 65 |
| Issue Number: | 20 |
| Collation: | 10 Seiten |
| DOI: | 10.1103/PhysRevB.65.205423 |
| Corresponding Links: | |
| 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. |
| Identification Number: | Artikel-ID: 205423 |
| Date Deposited: | 29 Oct 2010 10:00 |
| Last Modified: | 24 Apr 2024 14:35 |
| PPN: | |
| Export: | |
| Suche nach Titel in: | TUfind oder in Google |
Available Versions of this Item
-
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 Oct 2010 10:00) [Currently Displayed]
 |
Send an inquiry |
Options (only for editors)
 |
Show editorial Details |
Drucken
Impressum