Resonant molecular transitions in second harmonic generation spectroscopy of Fe-octaethylporphyrin adsorbed on Cu(001)
Fuente:
arXiv
Gespeichert in:
| Hauptverfasser: | , , , , , , |
|---|---|
| Format: | Preprint |
| Veröffentlicht: |
2024
|
| Schlagworte: | |
| Online-Zugang: | |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| _version_ | 1866909316909367296 |
|---|---|
| author | Eschenlohr, A. Shi, R. Chen, J. Zhou, P. Bovensiepen, U. Hübner, W. Lefkidis, G. |
| author_facet | Eschenlohr, A. Shi, R. Chen, J. Zhou, P. Bovensiepen, U. Hübner, W. Lefkidis, G. |
| contents | Metal-organic molecular adsorbates on metallic surfaces offer the potential to both generate materials for future (spin-)electronics applications as well as a better fundamental understanding of molecule-substrate interaction, provided that the electronic properties of such interfaces can be analyzed and/or manipulated in a targeted manner. To investigate electronic interactions at such interfaces, we measure optical second harmonic generation (SHG) from iron-octaethylporphyrin (FeOEP) adsorbed on Cu(001), and perform electronic structure calculations using coupled cluster methods including optical excitations. We find that the SHG response of FeOEP/Cu(001) is modified at 2.15-2.35 eV fundamental photon energy compared to the bare Cu(001) surface. Our polarization-dependent analysis shows that the $χ_{zzz}^{(2)}$ non-linear susceptibility tensor element dominates this modification. The first-principles calculations confirm this effect and conclude a resonantly enhanced SHG by molecular transitions at $\hbarω\geq 2$ eV. We show that the enhancement of $χ^{(2)}_{zzz}$ results from a strong charge-transfer character of the molecule-substrate interaction. Our findings demonstrate the suitability of surface SHG for the characterization of such interfaces and the potential to employ it for time-resolved SHG experiments on optically induced electronic dynamics. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2409_09801 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Resonant molecular transitions in second harmonic generation spectroscopy of Fe-octaethylporphyrin adsorbed on Cu(001) Eschenlohr, A. Shi, R. Chen, J. Zhou, P. Bovensiepen, U. Hübner, W. Lefkidis, G. Materials Science Chemical Physics Metal-organic molecular adsorbates on metallic surfaces offer the potential to both generate materials for future (spin-)electronics applications as well as a better fundamental understanding of molecule-substrate interaction, provided that the electronic properties of such interfaces can be analyzed and/or manipulated in a targeted manner. To investigate electronic interactions at such interfaces, we measure optical second harmonic generation (SHG) from iron-octaethylporphyrin (FeOEP) adsorbed on Cu(001), and perform electronic structure calculations using coupled cluster methods including optical excitations. We find that the SHG response of FeOEP/Cu(001) is modified at 2.15-2.35 eV fundamental photon energy compared to the bare Cu(001) surface. Our polarization-dependent analysis shows that the $χ_{zzz}^{(2)}$ non-linear susceptibility tensor element dominates this modification. The first-principles calculations confirm this effect and conclude a resonantly enhanced SHG by molecular transitions at $\hbarω\geq 2$ eV. We show that the enhancement of $χ^{(2)}_{zzz}$ results from a strong charge-transfer character of the molecule-substrate interaction. Our findings demonstrate the suitability of surface SHG for the characterization of such interfaces and the potential to employ it for time-resolved SHG experiments on optically induced electronic dynamics. |
| title | Resonant molecular transitions in second harmonic generation spectroscopy of Fe-octaethylporphyrin adsorbed on Cu(001) |
| topic | Materials Science Chemical Physics |
| url | https://arxiv.org/abs/2409.09801 |