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Vibronic enhancement of excitation energy transport: Interplay between local and non-local exciton-phonon interactions
- Source :
- The Journal of Chemical Physics. 146:075101
- Publication Year :
- 2017
- Publisher :
- AIP Publishing, 2017.
-
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 interactions. 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 a 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.
- Subjects :
- 010304 chemical physics
Chemistry
Phonon
Quantum dynamics
Exciton
General Physics and Astronomy
02 engineering and technology
021001 nanoscience & nanotechnology
01 natural sciences
Vibronic coupling
symbols.namesake
Franck–Condon principle
0103 physical sciences
symbols
Vibronic spectroscopy
Physics::Chemical Physics
Physical and Theoretical Chemistry
Atomic physics
0210 nano-technology
Hamiltonian (quantum mechanics)
Excitation
Subjects
Details
- ISSN :
- 10897690 and 00219606
- Volume :
- 146
- Database :
- OpenAIRE
- Journal :
- The Journal of Chemical Physics
- Accession number :
- edsair.doi.dedup.....7e5267b70eb0f46a7520c3934eb88e2b
- Full Text :
- https://doi.org/10.1063/1.4976558