Cavity-Mediated Enhancement of the Energy Transfer in the Reduced Fenna–Matthews–Olson Complex
Date
2024-08-27
Journal Title
Journal ISSN
Volume Title
Publisher
Journal of Chemical Theory and Computation
Abstract
Strong light-matter interaction leads to the formation of hybrid polariton states and can alter the light-harvesting properties of natural photosynthetic systems without modifying their chemical structure. In the present study, we computationally investigate the effect of the resonant cavity on the efficiency and the rate of the population transfer in a quantum system coupled to the cavity and the dissipative environment. The parameters of the model system were chosen to represent the Fenna–Matthews–Olson natural light-harvesting complex reduced to the three essential sites. The dynamics of the total system was propagated using the hierarchical equations of motion. Our results show that the strong light-matter interaction can accelerate the population transfer process compared to the cavity-free case but at the cost of lowering the transfer efficiency. The transition to the strong coupling regime was found to coincide with the degeneracy of polariton eigenvalues. Our findings indicate the potential and the limit of tuning the energy transfer in already efficient natural light-harvesting systems.
Description
This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Chemical Theory and Computation, copyright © 2024 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jctc.4c00626.
This article will be embargoed until 08/27/2025.
Keywords
cavities, energy, energy transfer, polaritons, quantum mechanics
Citation
Herrera Rodríguez, Luis E., Aarti Sindhu, Kennet J. Rueda Espinosa, and Alexei A. Kananenka. “Cavity-Mediated Enhancement of the Energy Transfer in the Reduced Fenna–Matthews–Olson Complex.” Journal of Chemical Theory and Computation 20, no. 17 (September 10, 2024): 7393–7403. https://doi.org/10.1021/acs.jctc.4c00626.