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Dark states and delocalization: Competing effects of quantum coherence on the efficiency of light harvesting systems

Natural light harvesting systems exploit electronic coupling of identical chromophores to generate efficient and robust excitation transfer and conversion. Dark states created by strong coupling between chromophores in the antenna structure can significantly reduce radiative recombination and enhance energy conversion efficiency. Increasing the number of the chromophores increases the number of dark states and the associated enhanced energy conversion efficiency yet also delocalizes excitations away from the trapping center and reduces the energy conversion rate. Therefore, a competition between dark state protection and delocalization must be considered when designing the optimal size of a light harvesting system. In this study, we explore the two competing mechanisms in a chain-structured antenna and show that dark state protection is the dominant mechanism, with an intriguing dependence on the parity of the number of chromophores. This dependence is linked to the exciton distribution among eigenstates, which is strongly affected by the coupling strength between chromophores and the temperature. Combining these findings, we propose that increasing the coupling strength between the chromophores can significantly increase the power output of the light harvesting system.
- Purdue University West Lafayette United States
- Qatar Airways United States
- Hamad bin Khalifa University Qatar
- TRUSTEES OF PURDUE UNIVERSITY United States
- Hamad bin Khalifa University Qatar
Chemical Physics (physics.chem-ph), Light-Harvesting Protein Complexes, FOS: Physical sciences, Pigments, Biological, Energy Transfer, Physics - Chemical Physics, Quantum Theory, Photosynthesis, Physics - Optics, Optics (physics.optics)
Chemical Physics (physics.chem-ph), Light-Harvesting Protein Complexes, FOS: Physical sciences, Pigments, Biological, Energy Transfer, Physics - Chemical Physics, Quantum Theory, Photosynthesis, Physics - Optics, Optics (physics.optics)
citations This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).21 popularity This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.Top 10% influence This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).Average impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.Top 10%
