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Intramolecular vibrations enhance the quantum efficiency of excitonic energy transfer

  • We study the impact of underdamped intramolecular vibrational modes on the efficiency of the excitation energy transfer in a dimer in which each state is coupled to its own underdamped vibrational mode and, in addition, to a continuous background of environmental modes. For this, we use the numerically exact hierarchy equation of motion approach. We determine the quantum yield and the transfer time in dependence of the vibronic coupling strength, and in dependence of the damping of the incoherent background. Moreover, we tune the vibrational frequencies out of resonance with the excitonic energy gap. We show that the quantum yield is enhanced by up to 10% when the vibrational frequency of the donor is larger than at the acceptor. The vibronic energy eigenstates of the acceptor acquire then an increased density of states, which leads to a higher occupation probability of the acceptor in thermal equilibrium. We can conclude that an underdamped vibrational mode which is weakly coupled to the dimer fuels a faster transfer of excitation energy, illustrating that long-lived vibrations can, in principle, enhance energy transfer, without involving long-lived electronic coherence.

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Author:Hong-Guang Duan, Peter Nalbach, R. J. Dwayne Miller, Michael Thorwart
Parent Title (English):Photosynthesis Research
Document Type:Article
Date of Publication (online):2021/01/15
Year of first Publication:2020
Publishing Institution:Westfälische Hochschule Gelsenkirchen Bocholt Recklinghausen
Release Date:2021/01/15
Tag:efficiency of exciton transfer; excitation energy transfer; vibronic coupling
First Page:137
Last Page:145
Departments / faculties:Fachbereiche / Wirtschaft und Informationstechnik Bocholt
Licence (German):License LogoEs gilt das Urheberrechtsgesetz

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