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Vibration-Assisted and Vibration-Hampered Excitonic Quantum Transport.
Journal of Physical Chemistry Letters 2018 June 8
The interplay between excitons and vibrations is considered to be a key factor in determining the exciton-transfer properties in light-harvesting complexes. Here we study this interplay theoretically in a model for exciton transport, composed of two chromophores coupled to an exciton source and sink in the presence of vibrations. We consider two cases that show qualitatively distinct transport features. In the first, the vibrations are global and affect the two chromophores simultaneously. In the second case, the vibrations are localized on each chromophore. For global vibrations, the current exhibits antiresonances as a function of the chromophore energy difference, which are due to exciton-polaron interference. For local vibrations, on the contrary, the currents show tunneling resonances at multiples of the vibration energy. Counterintuitively, both effects increase with increasing temperature. Our results demonstrate that an environment can either assist or hamper exciton transport and is in accord with the current understanding of energy transfer in natural exciton-transfer complexes.
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