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Vibronic enhancement of excitation energy transport : interplay between local and non-local exciton-phonon interaction
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Lee, Myeong H. and Troisi, Alessandro (2017) Vibronic enhancement of excitation energy transport : interplay between local and non-local exciton-phonon interaction. Journal of Chemical Physics, 146 (7). 075101.
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WRAP_1373481-ch-110217-vibronic_resonance.pdf - Accepted Version - Requires a PDF viewer. Download (885Kb) | Preview |
Official URL: http://dx.doi.org/10.1063/1.4976558
Abstract
It has been reported in recent years that vibronic resonance between vibrational energy of the intramolecular nuclear mode and excitation-energy difference is crucial to enhance excitation energy transport in light harvesting proteins. Here we investigate how vibronic enhancement induced by vibronic resonance is influenced by the details of local and non-local exciton-phonon interaction. We study a heterodimer model with parameters relevant to the light-harvesting proteins with the surrogate Hamiltonian quantum dynamics method in a vibronic basis. In addition, the impact of field-driven excitation on the efficiency of population transfer is compared with the instantaneous excitation, and the effect of multi-mode vibronic coupling is presented in comparison with the coupling to a single effective vibrational mode. We find that vibronic enhancement of site population transfer is strongly suppressed with the increase of non-local exciton-phonon interaction and increasing the number of strongly coupled high-frequency vibrational modes leads to further decrease in vibronic enhancement. Our results indicate that vibronic enhancement is present but may be much smaller than previously thought and therefore care needs to be taken when interpreting its role in excitation energy transport. Our results also suggest that non-local exciton-phonon coupling, which is related to the fluctuation of the excitonic coupling, may be as important as local exciton-phonon coupling and should be included in any quantum dynamics model.
| Item Type: | Journal Article | ||||||
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| Subjects: | Q Science > QC Physics | ||||||
| Divisions: | Faculty of Science > Chemistry | ||||||
| Library of Congress Subject Headings (LCSH): | Exciton theory, Phonons, Energy transfer | ||||||
| Journal or Publication Title: | Journal of Chemical Physics | ||||||
| Publisher: | American Institute of Physics | ||||||
| ISSN: | 0021-9606 | ||||||
| Official Date: | 21 February 2017 | ||||||
| Dates: |
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| Volume: | 146 | ||||||
| Number: | 7 | ||||||
| Article Number: | 075101 | ||||||
| Status: | Peer Reviewed | ||||||
| Publication Status: | Published | ||||||
| Funder: | European Research Council (ERC) | ||||||
| Grant number: | Grant No. 615834 |
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