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- Title
Interplay between structural hierarchy and exciton diffusion in artificial light harvesting.
- Authors
Kriete, Björn; Lüttig, Julian; Kunsel, Tenzin; Malý, Pavel; Jansen, Thomas L. C.; Knoester, Jasper; Brixner, Tobias; Pshenichnikov, Maxim S.
- Abstract
Unraveling the nature of energy transport in multi-chromophoric photosynthetic complexes is essential to extract valuable design blueprints for light-harvesting applications. Long-range exciton transport in such systems is facilitated by a combination of delocalized excitation wavefunctions (excitons) and exciton diffusion. The unambiguous identification of the exciton transport is intrinsically challenging due to the system's sheer complexity. Here we address this challenge by employing a spectroscopic lab-on-a-chip approach: ultrafast coherent two-dimensional spectroscopy and microfluidics working in tandem with theoretical modeling. We show that at low excitation fluences, the outer layer acts as an exciton antenna supplying excitons to the inner tube, while under high excitation fluences the former converts its functionality into an exciton annihilator which depletes the exciton population prior to any exciton transfer. Our findings shed light on the excitonic trajectories across different sub-units of a multi-layered artificial light-harvesting complex and underpin their great potential for directional excitation energy transport. Light-harvesting antennas and efficient energy transfer enable photosynthesis in low light conditions in natural systems. Here the authors resolve exciton properties and the role of structural hierarchy in a model light-harvesting complex by excited-state 2D spectroscopy on a microfluidic platform.
- Subjects
DIFFUSION; ENERGY transfer; MICROFLUIDICS; HARVESTING
- Publication
Nature Communications, 2019, Vol 10, Issue 1, pN.PAG
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-019-12345-9