Unraveling the Mechanism of Tip-Enhanced Molecular Energy Transfer
Fuente:
arXiv
Saved in:
| Main Authors: | , , , , |
|---|---|
| Format: | Preprint |
| Published: |
2023
|
| Subjects: | |
| Online Access: | |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866911769354567680 |
|---|---|
| author | Coane, Colin Romanelli, Marco Dall'Osto, Giulia Di Felice, Rosa Corni, Stefano |
| author_facet | Coane, Colin Romanelli, Marco Dall'Osto, Giulia Di Felice, Rosa Corni, Stefano |
| contents | Electronic Energy Transfer (EET) between chromophores is fundamental in many natural light-harvesting complexes, serving as a critical step for solar energy funneling in photosynthetic plants and bacteria. The complicated role of the environment in mediating this process in natural architectures has been addressed by recent scanning tunneling microscope (STM) experiments involving EET between two molecules supported on a solid substrate. These measurements demonstrated that EET in such conditions has peculiar features, such as a steep dependence on the donor-acceptor distance, reminiscent of a short-range mechanism more than of a Forster-like process. By using state of the art hybrid ab initio electromagnetic modeling, here we provide a comprehensive theoretical analysis of tip-enhanced EET. In particular, we show that this process can be understood as a complex interplay of electromagnetic-based molecular plasmonic processes, whose result may effectively mimic short range effects. Therefore, the established identification of an exponential decay with Dexter-like effects does not hold for tip-enhanced EET, and accurate electromagnetic modeling is needed to identify the EET mechanism. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2305_17265 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Unraveling the Mechanism of Tip-Enhanced Molecular Energy Transfer Coane, Colin Romanelli, Marco Dall'Osto, Giulia Di Felice, Rosa Corni, Stefano Chemical Physics Electronic Energy Transfer (EET) between chromophores is fundamental in many natural light-harvesting complexes, serving as a critical step for solar energy funneling in photosynthetic plants and bacteria. The complicated role of the environment in mediating this process in natural architectures has been addressed by recent scanning tunneling microscope (STM) experiments involving EET between two molecules supported on a solid substrate. These measurements demonstrated that EET in such conditions has peculiar features, such as a steep dependence on the donor-acceptor distance, reminiscent of a short-range mechanism more than of a Forster-like process. By using state of the art hybrid ab initio electromagnetic modeling, here we provide a comprehensive theoretical analysis of tip-enhanced EET. In particular, we show that this process can be understood as a complex interplay of electromagnetic-based molecular plasmonic processes, whose result may effectively mimic short range effects. Therefore, the established identification of an exponential decay with Dexter-like effects does not hold for tip-enhanced EET, and accurate electromagnetic modeling is needed to identify the EET mechanism. |
| title | Unraveling the Mechanism of Tip-Enhanced Molecular Energy Transfer |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2305.17265 |